I think the $S_5$ work is correct (sorry, haven't looked at the $A_5$ work). I would do it a somewhat different way:
Since 5, but not 25, divides 120 (the size of $S_5$), the Sylow-5 subgroups of $S_5$ must be cyclic of order 5. There are 24 5-cycles in $S_5$, 4 of them in each of these subgroups, so, 6 Sylow-5 subgroups.
Similarly, the Sylow-3 subgroups must be cyclic of order 3. There are 20 3-cycles in $S_5$, 2 to a subgroup, so 10 Sylow-3 subgroups.
Since 8, but not 16, divides 120, the Sylow-2 subgroups must have order 8. Now, $S_4$ contains three copies of the dihedral group of order 8, and $S_5$ contains 5 copies of $S_4$, so I get 15 Sylow-2 subgroups.
Something like this ought to work for $A_5$.
EDIT: I think OP wants me to elaborate on the dihedral-group part of the argument.
Take a square, label its vertices, cyclically, with 1, 2, 3, 4. Then the element $(1234)$ of $S_4$ has a natural interpretation as the rotation, one-fourth of the way around, of the square, and the element $(13)$ is the flip in the diagonal through 2 and 4, so these two elements of $S_4$ generate a subgroup isomorphic to the dihedral group of order 8.
The same is true for the elements $(1342)$ and $(14)$, and also for the elements $(1423)$ and $(12)$, and those are the three copies of the dihedral group in $S_4$.
Now if you pick any one of the numbers 1, 2, 3, 4, 5, and consider all the elements of $S_5$ that fix that number, you get a subgroup of $S_5$ isomorphic to $S_4$. Those are your five copies of $S_4$ in $S_5$.
As was remarked before, you do not have to assume that $G \cong A_5$.
(1) You did that one correctly!
(2) If $|Syl_3(G)|=4$, and $S \in Syl_3(G)$, then $|G:N_G(S)|=4$. Now let $G$ act on the left cosets of $N_G(S)$ by left multiplication, then the kernel of this action is $core_G(N_G(S))=\bigcap_{g \in G}N_G(S)^g$, which is a normal subgroup. Hence, by the simplicity of $G$, it must be trivial and $G$ can embedded in $S_4$, a contradiction, since $60 \nmid 24$.
(3) We prove that if a non-abelian simple $G$, with $|G|=60$, has an abelian subgroup of order $6$, then $G \cong A_5$. This gives a contradiction, since it is easily seen that $A_5$ does not contain any elements of order $6$ (note that an abelian group of order $6$ must be cyclic).
So assume $H \lt G$ is abelian and $|H|=6$. $H$ is not normal so, $N_G(H)$ is a proper subgroup (if not then $H$ would be normal) and since $|G:N_G(H)| \mid 10$, we must have $|G:N_G(H)|=5$ ($=2$ is not possible since subgroups of index $2$ are normal). Similarly as in (2), $G/core_G(N_G(H))$ embeds homomorphically in $S_5$ this time. Of course $core_G(N_G(H))=1$, so $G$ is isomorphic to a subgroup of $S_5$ and since it is simple it must be isomorphic to $A_5$ (if we write also $G$ for the image in $S_5$, consider $G \cap A_5 \lhd G$ and use $|S_5:A_5|=2$).
(4) In general: if $G$ is a group with a unique element $x$ of order $2$, then $x \in Z(G)$. Why? Because for every $g \in G$, $g^{-1}xg$ has also order $2$ and must be equal to $x$. In your case $G$ is non-abelian simple, so $Z(G)=1$.
So only (1) is the true statement.
Edit For case (3) I forgot the case where $|G:N_G(H)|=10$. I have a proof that is quite sophisticated and maybe there is an easier way.
Anyway, in this case $H=N_G(H)$. Consider the subgroup $P$ of order $3$ of $H$. This must be a Sylow $3$-subgroup of $G$, since $3$ is the higest power of $3$ dividing $|G|=60$. Observe that in fact $N_G(P)=H$. This follows from what we showed in (2): $|Syl_3(G)|=|G:N_G(P)|=10$ and of course $H \subseteq N_G(P)$.
Trivially, $P \subset Z(N_G(P))$. Now $P$ satifies the criterion of Burnside's Normal $p$-Complement Theorem, see for example Theorem (5.13) here. But then $P$ has a normal complement $N$, such that $G=PN$ and $P \cap N=1$. Now $G$ is non-abelian simple, so $N=1$ or $N=G$, which both lead to a contradiction.
Best Answer
You could argue as follows, since Sylow subgroups are permuted transitively under conjugation.
If the number of Sylow $3$-subgroups is $4$, then they are permuted transitively by conjugation, and this gives rise to a non-trivial homomorphism to $S_4$. But $S_4$ has order $24\lt 60$ so such a homomorphism would have a non-trivial kernel.