Let's look at the function $$S(x)=\sum_{\begin{array}{c}
m,n\leq x\\
\gcd(m,n)=1\end{array}}1.$$
Then notice that $$S(x)=\sum_{m,n\leq x}\sum_{d|\gcd(m,n)}\mu(d)=\sum_{d\leq x}\sum_{r,s\leq\frac{x}{d}}\mu(d)= \sum_{d\leq x}\mu(d)\left[\frac{x}{d}\right]^{2}$$
From here it is straight forward to see that in the limit, $$\frac{S(x)}{x^2}\rightarrow\sum_{n=1}^\infty \frac{\mu(n)}{n^2}=\frac{1}{\zeta(2)}=\frac{6}{\pi^2}.$$
However, there are still some interesting questions here. How fast does in converge, and what are the secondary terms? It turns out we can easily relate this to the summatory totient function, which has a rich history. See these two math stack exchange posts: Totient function, Asymptotic formula. What follows below is a modification of
my answer on the second post.
The History Of The Error Term
In 1874, Mertens proved that $$S(x)=\frac{6}{\pi^{2}}x^{2}+O\left(x\log x\right).$$ Throughout we use $E(x)=S(x)-\frac{6}{\pi^2}x^2$ for the error function.
The best unconditional result is given by Walfisz 1963: $$E(x)\ll x\left(\log x\right)^{\frac{2}{3}}\left(\log\log x\right)^{\frac{4}{3}}.$$
In 1930, Chowla and Pillai showed this cannot be improved much more, and that $E(x)$ is not $$o\left(x\log\log\log x\right).$$
In particular, they showed that $\sum_{n\leq x}E(n)\sim\frac{3}{\pi^{2}}x^{2}$ so that $E(n)\asymp n$ on average. In 1950, Erdos and Shapiro proved that there exists $c$ such that for infinitely many positive integers $N,M$ we have $$E(N)>cN\log\log\log\log N\ \ \text{and}\ \ E(M)<-cM\log\log\log\log M, $$
or more concisely
$$E(x)=\Omega_{\pm}\left(x\log\log\log\log x\right).$$
In 1987 Montgomery improved this to
$$E(x)=\Omega_{\pm}\left(x\sqrt{\log\log x}\right).$$
Hope you enjoyed that,
Added: At some point, I wrote a long blog post about this, complete with a proof of Montgomery's lower bound.