We present ab-initio calculations of the independent components of gradient elastic tensors, so-called gradient elastic constants, which relate electric field gradient tensors to stress or strain tensors. The constants of cubic and hexagonal metals, MAX phases, and zinc oxide were determined within the framework of density functional theory by using the augmented plane waves plus local orbitals method implemented in the WIEN2k code. Comparison with experimental gradient elastic constants and electric field gradients' stress dependencies suggest an accuracy of about 30% of the calculated constants, independent of the probe that detects the field gradient being self- or foreign-atom. Changes in the electric field gradient take place by strain-induced asymmetric occupations of the p and d states in the valence region for all investigated materials. Volume and structural dependencies of the electric field gradient can directly be determined from this fundamental approach and are, for hexagonal closed packed metals, consistent with vanishing electric field gradients around ideal close packing and volume dependencies larger than one. The concept of these calculations is applicable in any hyperfine interaction method and, thus, can be used to gain information about intrinsic strains in systems where the experimental gradient elastic constants are inaccessible.