Composing two bijections is a bijection (when domains and codomains match up), and composing two homomorphisms is a homomorphism, so $\text{Aut}(G)$ is closed under associative function composition. And $g \mapsto g$ is an automorphism, and the inverse of an isomorphism is also an isomorphism, so $\text{Aut}(G)$ is a group. It is a subset of all the permutations of $G$ as a set, so if $|G| = n < \infty$, then $\text{Aut}(G) \leq S_n$. "The automorphism group is a subgroup of $S_n$."
However, we can't go the other way around. Given $S_n$, it doesn't make sense to say "this subgroup of $S_n$ is the automorphism group", because we need to specify "is an automorphism group with respect to..." some group $G$. Although, since there is only one automorphism group for a given group $G$, we could also say "is the automorphism group of $G$".
This distinction confused me a lot when I first thought about it. It also leads to a question: is there a "nice" description of each subgroup of $S_n$ (say, each subgroup of $S_6$) as the automorphism group of some well-known group? Of course, we will need a few different groups to accomplish this.
Related: Realizable automorphism groups of graphs
EDIT: Based on the comments, this question is very general and difficult. To make it answerable, I will narrow the scope. Are there any algorithms, theorems, or insights related to the following problem? Solving it is too much to ask, but I'd be happy to hear how one might begin to approach this task.
Given a finite group $H$ of reasonably small order, find a group $G$ such that $H \cong \text{Aut}(G)$.