Proton-detected solid-state NMR has emerged as a powerful analytical technique in structural elucidation via 1H-1H correlations, which are mostly established by broadband methods. We propose a new class of frequency-selective homonuclear recoupling methods to selectively enhance 1H-1H correlations of interest under ultrafast magic-angle spinning (MAS). These methods, dubbed as selective phase-optimized recoupling (SPR), can provide a sensitivity enhancement by a factor of ∼3 over the widely used radio-frequency-driven recoupling (RFDR) to observe 1HN-1HN contacts in a protonated tripeptide N-formyl-Met-Leu-Phe (fMLF) under 150 kHz MAS and are successfully utilized to probe a long-range 1H-1H contact in a pharmaceutical molecule, the hydrochloride form of pioglitazone (PIO-HCl). SPR is not only highly efficient in frequency-selective recoupling but also easy to implement, imparting to it great potential to probe 1H-1H contacts for the structural elucidation of organic solids such as proteins and pharmaceuticals under ultrafast MAS conditions.