Abstract Synchronized optical pulses are widely used. We report here characterization and measurement of synchronized femtosecond and picosecond pulses from a Ti:Sapphire laser (nominally 800 nm) and a Nd:YAG laser (1064 nm), respectively. Synchronization is achieved by utilizing soliton self-frequency shift in a photonic-crystal fiber that allows the 800 nm femtosecond oscillator to seed the third-harmonic generation (355 nm) of picosecond regenerative amplifier. The relative timing jitter between the amplified femtosecond and the third-harmonic generation of picosecond pulses is (710 ± 160) fs, which is only (1.17 ± 0.26)% of the picosecond pulse duration. This work paves way for applications in stimulated Raman scattering spectroscopy and amplification.