Note that $\overline{\lim} a_n$ and $\underline{\lim} a_n$ are always two particular subsequences of $(a_n)_n$.
If $a_n$ is bounded, these are monotonic sequences in a compact thus always converge.
So if you require that no two subsequences converge to different values, then it is also true for these two, and $\underline{\lim}=\overline{\lim}$ means $a_n$ converge.
Now if $a_n$ is not bounded, as stated there may not be converging subsequences [e.g. $a_n=n$].
Yet if you consider compactified $\mathbb R\cup\{-\infty,+\infty\}$ then the extended condition still impose $\underline{\lim}=\overline{\lim}$ so $a_n$ diverges to $\pm\infty$. This is a result stronger than just unbounded.