The question I was originally thinking about was:
Can $T_3$, the three-regular tree (the infinite tree with each vertex having valency 3) be the Cayley graph of some group with some generating set?
Since $T_2$ is $\text{Cay}(\mathbb Z, \{1\})$, and $T_4$ is $\text{Cay}(F_2=\langle a,b \rangle,\{a,b\})$, I thought for $T_3$ I could let $a,b,c$ be the three edges coming out of each vertex (in the case of $F_2$ the edges were $a,a^{-1},b,b^{-1}$ but here we can't get $3 $ edges if we allow inverses of the generators to be different from themselves).
So I think $T_3=\text{Cay}(\mathbb Z_2 * \mathbb Z_2 * \mathbb Z_2 , \{a,b,c\})$.
But now I could use the same logic and say $T_4= \text{Cay}(\mathbb Z_2 * \mathbb Z_2 * \mathbb Z_2 * \mathbb Z_2 , \{a,b,c,d\}) = \text{Cay}(F_2, \{s,t\})$.
Firstly, whatever I've written so far, is it at least correct?
If it is, can two non-isomorphic groups have the same Cayley graph?
(I think they can, because I really doubt $F_2 \cong \mathbb Z_2 * \mathbb Z_2 * \mathbb Z_2 * \mathbb Z_2$).

This answer assumes that by the Cayley graph $\operatorname{Cay}(G, S)$ you mean the directed and labelled graph with vertex set $G$ and where we can think of the edge set as the set of ordered triples $$\{(g,h,a)\in G\times G\times S\mid ga=h\}.$$ The fact that the triples are ordered corresponds to directed edges. The third component corresponds to a label on the edge.
This definition is the one I am most familiar with, and for example is used in Wikipedia.
It also assumes that by "graph" you allow multiple edges between any given two vertices (some texts call this a "multigraph"). If your definition of graph does not allow this, this your situation essentially reduces to my other answer.
By "removing labels" I mean forgetting the third component of each triple, and also the direction of each arrow, so the unlabelled Cayley graph is the multiset $$\{\{g,h\}\in G\times G\mid \exists\:a\in S\text{ s.t. }ga=h\}.$$ Being a multiset simply means we may have multiple edges between any two given vertices.
There are a few questions here. So lets answer them one-by-one.
If we remove the labels on edges, yes. The simplest family of examples is basically that pointed out by Sean Eberhard in the comments: For any group $G$, the Cayley graph $\operatorname{Cay}(G,G\setminus\{1\})$ is a complete graph but where every edge is replaced by two directed edges pointing in opposite directions. As there can be a great many groups of a given order (finite or infinite), this gives non-isomorphic groups with the same unlabelled Cayley graphs.
No. The Cayley graph looks like $T_3$, if you squint a little, but every edge $e=(u, v)$ has a "reversed" sibling $\bar{e}=(v, u)$ with the same label. The first edge means that $u\cdot a=v$ while the second means that $v\cdot a=u$, so in particular $u\cdot a^2=u$, which is what we'd expect as $a^2=1$.
Again, no. This is because a Cayley graph must have as many incoming edges as outgoing edges; in particular every vertex of $\operatorname{Cay}(G, S)$ has $|S|$ outgoing edges and $|S|$ incoming edges (why?). Hence, every vertex must have even degree. As vertices of $T_3$ have odd degree, it cannot be a Cayley graph.
[Fun fact: If a group acts freely on a tree then it is free. As groups act freely on their Cayley graphs, any group with a tree as its Cayley graph must actually be free. This wasn't used above, but is nice to know anyway :-) ]