Reformulate your set of equations such that the coefficients are the unknowns and perform least square fitting on A.
This can be done by the following trick:
Be $x$ a column vector $(n\times 1)$, $A$ the unknown matrix $(n\times n)$, you know that $Ax =b \Rightarrow \sum_j a_{ij} x_j = b_i$ but this can also be seen as $\hat X\, \textrm{Vec}(A)= b$ where $\textrm{Vec}(A)$ is the vectorization operator and $\hat X$ must be n-times repeated and shifted by n $x^T$ or $0^T$ otherwise, leading to $\Rightarrow \hat X=x^T\otimes I_n $, where $I_n$ is the identity matrix of dimension n.
For the full system you can rewrite it as following, set $X=(x_1,...,x_n)$ and $B=(b_1,...,b_n)$ of your original equations $A X = B$, your least square problem for $A$ reads $(X^T\otimes I_n)\textrm{Vec}(A)=\textrm{Vec}(B^T)$. (modulo some transpose, I might have missed$(X^T\otimes I_n)\textrm{Vec}(A)=\textrm{Vec}(B)$.)
So it all boils down if you have enough matrix equations whether this will be an over or undertemined system and can be directly solved by standard numerical techniques.