Ultrafast One-Dimensional Peierls-Distortion Dynamics in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow> <mml:mn>1</mml:mn> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi mathvariant="normal">T</mml:mi> </mml:mrow> <mm

Rhenium disulfide (ReS_{2}), a prototypical 2D semiconductor with an anisotropic 1T^{'} structure due to the pronounced Peierls distortion, has demonstrated great potential for polarization-dependent optoelectronics and photonics. Here, we report an ultrafast phase transition occurring within 1 ps, accompanied by a one-dimensional Peierls-distortion relaxation in 1T^{'}-ReS_{2} revealed with combined 4D electron microscopy and time-dependent density functional theory calculations. Upon femtosecond laser pulse excitation, the Re-Re dimerization morphology rapidly transforms from a diamond cluster to zigzag chains and persists for several nanoseconds. This ultrafast Peierls-distortion relaxation is further verified by transient changes in optical anisotropy via polarization-dependent transient absorption spectroscopy. Time-dependent density functional theory calculations attribute this novel phase transition to strong correlation between Peierls distortion and impulsive photoexcited carrier doping, predicting a transient band-gap collapse. This Letter opens up an exciting avenue for ultrafast control of Peierls-distortion-induced anisotropy and the metal-insulator transition in 1T^{'}-ReS_{2}.