These off-diagonal terms are called the products of inertia. If we have an angular velocity vector $\boldsymbol{\omega}$, then the product of inertia $I_{ij}$ is the proportionality constant that measures how much the $j$th component of $\boldsymbol{\omega}$ contributes to the $i$th component of the angular momentum. This is a simple generalization of normal moment of inertia $(I_{ii})$, which measures how much the $i$th component of angular velocity affects the $i$th component of the angular momentum.
The eigenvectors of this matrix describe the principal axes, which are the axes where, if you spin the object around one of these axes, the angular momentum will be parallel to the axis and the angular velocity. These axes are colinear with the eigenvectors. These axes are perpendicular, and thus we can use them as a basis for a coordinate system. If we do so, the inertia tensor becomes diagonalized. Each of the components on the diagonal axis are moments of inertia, and they will be the eigenvalues.