The cross-peak intensity for a S= 1/2, I= 1/2 spin system in two-dimensional HYSCORE spectra of single-crystals and powders is analyzed. There is a fundamental difference between these two cases. For single crystals, the cross-peak intensity is distributed between the two (+, +) and (+, −) quadrants of the hyperfine sublevel correlation (HYSCORE) spectrum by the ratio c2:s2(C. Gemperle, G. Aebli, A. Schweiger, and R. R. Ernst, J. Magn. Reson.88, 241 (1990)). However, for powder spectra another factor becomes dominant and governs cross-peak intensities in the two quadrants. This factor is the phase interference between modulation from different orientations of the paramagnetic species. This can lead to essentially complete disappearance of the cross-peak in one of the two (+, +) or (+, −) quadrants. In the (+, +) quadrant, cross-peaks oriented parallel to the main (positive) diagonal of the HYSCORE spectrum are suppressed, while the opposite is true in the (+, −) quadrant where cross-peaks nearly perpendicular to the main (negative) diagonal of HYSCORE spectra are suppressed. Analytical expressions are derived for the cross-peak intensity profiles in powder HYSCORE spectra for both axial and nonaxial hyperfine interactions (HFI). The intensity is a product of two terms, one depending only on experimental parameter (τ) and the other only on the spin Hamiltonian. This separation provides a rapid way to choose τ for maximum cross-peak intensity in a region of interest in the spectrum. For axial HFI, the Hamiltonian-dependent term has only one maximum and decreases to zero at the canonical orientations. For nonaxial HFI, this term produces three separate ridges which outline the whole powder lineshape. These three ridges have the majority of the intensity in the HYSCORE spectrum. The intensity profile of each ridge resembles that observed for axial HFI. Each ridge defines two principal values of the HFI similar to the ridges from an axial HFI.