Measurements of two-dimensional (2D) solid-state NMR spectra of homonuclear spin-1/2 pairs in stationary polycrystalline samples, reflecting dipolar and J couplings as well as anisotropic chemical shift interactions, are described. To obtain the correlation of the powder patterns in the 2D frequency plane, a pi-pulse spin-echo subsequence is incorporated into the evolution period of the 2D pulse sequence. In general, the spin-echo sequence does not perfectly refocus the influences of the chemical shift interactions, but such residual chemical shifts may cause complicated powder patterns in the relevant frequency dimension instead of the well-known Pake patterns. The analysis of the 2D spin-echo powder patterns thus obtained for P-31-P-31 systems in tetraphenyldiphosphine and sodium pyrophosphate decahydrate and a C-13-C-13 system in 1,2-C-13 doubly-labeled palmitic acid has yielded their spin parameters; in spectral simulations, the residual chemical shift effects play an important role in giving correct and, in some cases, otherwise unobtainable parameters. Information on molecular structures, such as internuclear directions with respect to the principal axis systems of the chemical shift tensors, has been obtained for the above compounds. In particular, the conformation of the molecules in the crystalline systems has been clarified and discussed in detail.