A high-speed, master-oscillator power-amplifier burst-mode laser with ∼100 ps pulse duration is demonstrated with output energy up to 110 J per burst at 1064 nm and second-harmonic conversion efficiency up to 67% in a KD*P crystal. The output energy is distributed across 100 to 10,000 sequential laser pulses, with 10 kHz to 1 MHz repetition rate, respectively, over 10 ms burst duration. The performance of the 100 ps burst-mode laser is evaluated and been found to compare favorably with that of a similar design that employs a conventional ∼8 ns pulse duration. The nearly transform-limited spectral bandwidth of 0.15 cm⁻¹ at 532 nm is ideal for a wide range of linear and nonlinear spectroscopic techniques, and the 100 picosecond pulse duration is optimal for fiber-coupled spectroscopic measurements in harsh reacting-flow environments.