Sensitivity is often a limiting factor in electron–nuclear double resonance (ENDOR). Here we demonstrate how using chirp radiofrequency pulses can improve ENDOR sensitivity up to 3–9 fold, with the strongest increase for broader lines often encountered in disordered solids for nuclei such as nitrogen and metals. The resulting drastic speedup in acquisition times also renders 2D ENDOR more feasible, as we demonstrate in TRIPLE, showing correlations with Cu hyperfine couplings.