We report the first excimer (XeF) pumping of Nd3+in a pentaphosphate (Nd : P5O14) host. Absorption of the XeF laser output of 3530 A˚ by the Nd3+transition (4I9/2→4D3/2) results in laser output at the 1.05‐&mgr; transition (4F3/2→4I11/2). Pumped in an oscillator configuration, threshold energy was only ≃3 mJ while slope efficiency was ≃1%. Temporal output consists of a single pulse of duration (FWHM) ≃6.6 ns; it arises due to the combination of short pump pulse (≃24 ns FWHM) and high gain of the pentaphosphate output. The device is expected to find considerable application in producing short (1–10 ns) pulses without the complication of aQswitch required in conventional flashlamp‐pumped lasers.