A new self-activated NdTaO4 (NTO) crystal with the size of 30 mm×60 mm is grown by Czochralski method, and its crystal structure is investigated by the Rietveld full-profile fitting method. The grown NTO crystal shows the monoclinic system, space group I2/a, and lattice constants and density are also given. The room temperature absorption and emission spectra of NTO crystal are studied. The strong broadband absorption peaks at 808.5 nm and 885 nm and the obvious broadband emission at 1063.5 nm are suitable for the laser diode (LD) pumped tunable laser or ultrashort laser. The NTO crystal can be used as a high gain self-activated microchip laser medium.