If $G$ is nilpotent, and $a$ and $b$ are element of relatively prime finite order, then $a$ and $b$ commute; this holds whether $G$ is finite or not. (That is, the condition is necessary, so "only if" holds in all cases).
Note. Plop's argument below is much easier than mine here. This is probably a result of When-You-Have-a-Hammer Syndrome. I've used commutator calculus a lot in my work, so it tends to be one of the first tools I reach for when dealing with these kinds of problems.
Since an element of finite order can be written as a product of elements of prime power order, it suffices to consider the case where $a$ and $b$ are of prime power order, $\mathrm{ord}(a) = p^n$, $\mathrm{ord}(b) = q^m$, $p$ and $q$ distinct primes, $n,m$ positive integers.
The key is to use the following consequences of P. Hall's collections process (you can see the basic results in Marshall Hall's Group Theory book; I'm quoting these theorems from R.R. Struik's Nilpotent products of cyclic groups, Canad. J. Math. 12 (1960), 447-462.
Theorem. Let $x$ and $y$ be any two elements of a group. Ldt $u_1,\ldots,u_n,\ldots$ be a fixed sequence of commutators in $x$ and $y$ of non-decreasing wight; that is, $u_1 = [x,y]$, $u_2=[[x,y],x]$, $u_3 = [[x,y],y]$, etc. Then $(xy)^n = x^ny^n u_1^{f_1(n)}u_2^{f_2(n)}\cdots u_t^{f_t(n)}\cdots$ where $f_i(n) = a_1\binom{n}{1}+a_2\binom{n}{2}+\cdots+a_{w_i}\binom{n}{w_i},$ $a_i$ are rational integers, and $w_ii$ is the weight of $u_i$ as a commutator in $x$ and $y$. The first formula is an identity if the group is nilpotent; otherwise, it can be considered as giving a series of approximations to $(xy)^n$ modulo successive terms of the lower central seres.
Theorem. Let $\alpha$ be a fixed integer, and let $G$ be a group such that the $n$th term of the loweer central series of $G$ is trivial. Then if $b_j\in G$ and $r\lt n$, $[b_1,\ldots,b_{i-1},b_i^{\alpha},b_{i+1},\ldots,b_r] = [b_1,\ldots,b_r]^{\alpha} v_1^{f_1(\alpha)}v_2^{f_2(\alpha)}\cdots$ where the $v_k$ are commutators in $b_1,\ldots,b_r$ of weight greater than $r$, and every $b_j$, $1\leq j\leq r$ appears in each commutator $v_k$. The $f_i$ are of the form $f_i(n) = a_1\binom{n}{1}+a_2\binom{n}{2}+\cdots+a_{w_i}\binom{n}{w_i}$ where $w_i$ is the weight of $v_i$ minus $r-1$.
Using these two theorems and decreasing induction, it is easy to verify that if $G$ is nilpotent, then for a sufficiently large power of $p$ we have $[a^{p^N},b] = [a,b^{p^N}].$ For a sufficiently large $N$, the left hand side is trivial; on the right hand side, since $b$ is of order prime to $p$, it follows that $b$ is a power of $p^N$, so the fact that $[a,b^{p^N}]$ is trivial, which is equivalent to the fact that $a$ commutes with $b^{p^N}$, implies that $a$ also commutes with any power of $b^{p^N}$, in particular that $a$ commutes with $b$.
So if $G$ is nilpotent, whether finite or infinite, and $a,b\in G$ are two elements of finite coprime order, then $a$ and $b$ commute.
The converse is true for finite groups (a finite group is nilpotent if and only if it is a direct product of $p$-groups, which implies that two elements of coprime order will commute. But the converse is false for infinite groups. In addition to Plop's example, here's a torsion example in which the condition is satisfied nonvacuously:
Fix a prime $p$. For each $n\gt 1$, let $G(p,n)$ be a nilpotent group of order $p^n$ and maximal class (that is, of class $n-1$); such groups exist. Let $\mathfrak{G}_p = \bigoplus_{n=2}^{\infty} G(p,n).$ Then $\mathfrak{G}_p$ is torsion, but is not nilpotent, since the $n$th term of the lower central series of $\mathfrak{G}_p$ is the direct sum of the $n$th terms of the lower central series of the $G(p,m)$ for each $m$, so it is not trivial for every $n$. Now take two distinct primes, $p$ and $q$, and let $\mathcal{G}=\mathfrak{G}(p)\oplus\mathfrak{G}(q)$. This is torsion, has nontrivial elements of coprime order, any two elements of coprime order commute, but $\mathcal{G}$ is not nilpotent (since it has non-nilpotent sugroups).
So the condition is necessary in general, and sufficient in the finite case for nilpotency.