We developed an optically synchronized highly stable frequency-doubled Nd:YAG laser with sub-nanosecond pulse duration. The 1064 nm seed pulses generated by soliton self-frequency shift in a photonic crystal fiber from Ti:sapphire oscillator pulses were stabilized by controlling input pulse polarization. The seed pulses were amplified to 200 mJ by diode-pumped amplifiers with a high stability of only <0.2% (rms). With an external LBO doubler, the system generated 330 ps green pulse energy of 130 mJ at 532 nm with a conversion efficiency of 65%. The pulse duration was further extended to 490 ps by adjusting Nd:YAG crystal temperature. To the best of our knowledge, these results present a longer pulse duration with higher stability than previous Nd:YAG lasers with sub-nanosecond optical synchronization.