Solid-state nuclear magnetic resonance (NMR) is a powerful and indispensable tool for structural and dynamic studies of various challenging systems. Nevertheless, it often suffers from significant limitations due to the inherent low signal sensitivity when low- nuclei are involved. Herein, we report an efficient solid-state NMR approach for rapid and efficient structural analysis of minute amounts of organic solids. By encoding staggered chemical shift evolution in the indirect dimension and staggered acquisition in 1H dimension, a proton-detected homonuclear 1H/1H and heteronuclear 13C/1H chemical shift correlation (HETCOR) spectrum can be obtained simultaneously in a single experiment at fast magic-angle-spinning (MAS) conditions with barely increasing experimental time, compared to conventional proton-detected HETCOR experiment. We establish that abundant 1H polarization can be efficiently manipulated and fully utilized in proton-detected solid-state NMR spectroscopy for extraction of more critical structural information and thus reduction of total experimental time.