The Eilenberg-Zilber theorem says that for singular homology there is a natural chain homotopy equivalence:
$$S_*(X)\otimes S_*(Y) \cong S_*(X\times Y)$$
The map in the reverse direction is the Alexander-Whitney map. Therefore we obtain a map
$$S_*(X)\rightarrow S_*(X\times X) \rightarrow S_*(X)\otimes S_*(X)$$
which makes $S_*(X)$ into a coalgebra.
My source (Selick's Introduction to Homotopy Theory) then states that this gives $H_*(X)$ the structure of a coalgebra. However, I think that the Kunneth formula goes the wrong way. The Kunneth formula says that there is a short exact sequence of abelian groups:
$$0\rightarrow H_*(C)\otimes H_*(D) \rightarrow H_*(C \otimes D) \rightarrow \operatorname{Tor}(H_*(C), H_*(D)) \rightarrow 0$$
(the astute will complain about a lack of coefficients. Add them in if that bothers you)
This is split, but not naturally, and when it is split it may not be split as modules over the coefficient ring. To make $H_*(X)$ into a coalgebra we need that splitting map. That requires $H_*(X)$ to be flat (in which case, I believe, it's an isomorphism).
That's quite a strong condition. In particular, it implies that cohomology is dual to homology.
Of course, if one works over a field then everything's fine, but then integral homology is so much more interesting than homology over a field.
In the situation for cohomology, only some of the directions are reversed, which means that the natural map is still from the tensor product of the cohomology groups to the cohomology of the product. Since the diagonal map now gets flipped, this is enough to define the ring structure on $H^*(X)$.
There are deeper reasons, though. Cohomology is a representable functor, and its representing object is a ring object (okay, graded ring object) in the homotopy category. That's the real reason why $H^*(X)$ is a ring (the Kunneth formula has nothing to do with defining this ring structure, by the way). It also means that cohomology operations (aka natural transformations) are, by the Yoneda lemma, much more accessible than the corresponding homology operations (I don't know of any detailed study of such).
Rings and algebras, being varieties of algebras (in the sense of universal or general algebra) are generally much easier to study than coalgebras. Whether this is more because we have a greater history and more experience, or whether they are inherently simpler is something I shall leave for another to answer. Certainly, I feel that I have a better idea of what a ring looks like than a coalgebra. One thing that makes life easier is that often spectral sequences are spectral sequences of rings, which makes them simpler to deal with - the more structure, the less room there is for things to get out of hand.
Added Later: One interesting thing about the coalgebra structure - when it exists - is that it is genuinely a coalgebra. There's no funny completions of the tensor product required. The comultiplication of a homology element is always a finite sum.
Two particularly good papers that are worth reading are the ones by Boardman, and Boardman, Johnson, and Wilson in the Handbook of Algebraic Topology. Although the focus is on operations of cohomology theories, the build-up is quite detailed and there's a lot about general properties of homology and cohomology theories there.
Added Even Later: One place where the coalgebra structure has been extremely successfully exploited is in the theory of cohomology cooperations. For a reasonable cohomology theory, the cooperations (which are homology groups of the representing spaces) are Hopf rings, which are algebra objects in the category of coalgebras.
Grothendieck's Tohoku paper was an attempt to set the foundations of algebraic topology on a uniform basis, essentially to describe a setting where one can do homological algebra in a way that makes sense. He did this by using the concept of abelian categories. Perhaps a better question to ask yourself is "Why are abelian categories a good idea?" In answering your question, I will do some major handwaving and sacrifice some rigor for the sake of clarity and brevity, but will try to place the Tohoku paper in context.
At the time, the state-of-the-art in homological algebra was relatively primitive. Cartan and Eilenberg had only defined functors over modules. There were some clear parallels with sheaf cohomology that could not be mere coincidence, and there was a lot of evidence that their techniques worked in more general cases. However, in order to generalize the methodology from modules, we needed the category in question to have some notion of an exact sequence. This is a lot trickier than it might seem. There were many solid attempts to do so, and the Tohoku paper was a giant step forward in the right direction.
In a nutshell, Grothendieck was motivated by the idea that $Sh(X)$, the category of sheaves of abelian groups on a topological space $X$ was an abelian category with enough injectives, so sheaf cohomology could be defined as a right-derived functor of the functor of global sections. Running with this concept, he set up his famous axioms for what an abelian category might satisfy.
Using the framework given by these axioms, Grothendieck was able to generalize Cartan and Eilenberg's techniques on derived functors, introducing ideas like $\delta$-functors and $T$-acyclic objects in the process. He also introduces an important computational tool, what is now often called the Grothendieck spectral sequence. This turns out to generalize many of the then-known spectral sequences, providing indisputable evidence that abelian categories are the "right" setting in which one can do homological algebra.
However, even with this powerful new context, there were many components missing. For instance, one couldn't even chase diagrams in general abelian categories using the techniques from Tohoku in and of itself, because it did not establish that the objects that you wanted to chase even existed. It wasn't until we had results like the Freyd-Mitchell embedding theorem that useful techniques like diagram chasing in abelian categories became well-defined. Henceforth, one had a relatively mature theory of homological algebra in the context of abelian categories, successfully generalizing the previous methods in homological algebra. In other words, we have "re-interpreted the basics of [algebraic] topology" by allowing ourselves to work with the more general concept of abelian categories.
Best Answer
It is somewhat jarring to hear of people who "know nothing about the homology theories of topological spaces and their applications" but are "familiar with homological algebra, category theory, spectral sequences (!!)" and the like. Certainly, this is a historically backwards position to be in, since a lot of these highly abstract theories with which you are familiar were almost entirely motivated by the concrete theory which you now wish to master.
Based on what you have said about your background, you will find Peter May's book "A Concise Course in Algebraic Topology" an appropriate read. Peter does not shy away from using categorical or homological machinery when dealing with this material, but also encourages his reader to become adept at the sort of calculations which yield insight into the nature of the subject. Amazingly, you can get the book freely off his website.
Also, to really hammer in the fact that you are engaging with a living, breathing, highly applicable subject, check out Kaczynski, Mischaikow and Mrozek's "Computational Homology" and Edelsbrunner and Harer's "Computational Topology" to find a breadth of applications of homology to physical and life sciences.
Update: The OP and others in a similar position may also be interested in my own upcoming book. You can find the cover here.