Through two-photon lithographic processes, we report experimentally and numerically a series of photoinduced tunable polymerization patterns in shapes from straight channel, serpentine curve, to periodic grating when an ultrashort femtosecond laser pulse directly writes in a liquid-crystal-monomer mixture along a line for different scanning speeds. Laser beams with polarization perpendicular to the direction of writing and the alignment of liquid crystals, produce snake-shaped patterns at an intermediate scan rate [2][3][4][5]. In comparison to one-photon absorption, in recent decades, two-photon (TP) lithography has emerged as a promising technique for direct laser writing, for its capacity to fabricate fine and well formed patterns, as well as three-dimensional structures, microscaled in size and nanoscaled in resolution [6,7]. Commercially available photopolymerizable monomers are generally transparent to infrared light and allow a deeper penetration, which makes them excellent candidates for two-photon polymerization (TPP). Although TP direct laser writing has been widely used for local alignment of LCs in predetermined structures like gratings, it has not been directly used to demonstrate transition of written patterns. Such transitional patterns have been observed in several hydrodynamic systems exhibiting symmetry-braking instabilities, resulting in patterns like coiling, buckling of jets, and meandering [8][9][10]. In this work, by scanning the laser along a straight line, formation and transition of various structures in the form of straight waveguide, serpentine patterns, and microgratings are demonstrated experimentally, through the TPP lithography in PDLCs by varying only the scanning speed of the laser. The direction of polarization of the writing beam plays an important role in the formation of curved structures, for which an original sinusoidally modulated laser intensity is transferred into a curved serpentine shape. Optical images taken from parallel and perpendicular analyzers reveal the reorientation of LCs, and a theoretical model with the introduction of convection flow is developed to explain these observed symmetry-breaking structures. The experimental setup for the fabrication is illustrated in Fig. 1. The LC-monomer mixture consisting of 30 wt. % of nematic LC E7 [11,12], 69.4 wt. % monomer NOA65 (Norland), 0.5 wt. % photoinitiator Rose bengal (Oregon medical laser center), and 0.1 wt. % of dye bis (2,4,6-trimethylbenzoy) phenylphosphine oxide (Ciba: Irgacure 819) is sandwiched between two glass slides with a separation of 30 μm. The glass surfaces are treated with DMOAP (N, N-dimethyl-Noctadecyl-3-aminopropyl-trimethoxysilyl chloride 6), in order to let the LC molecules stay in a hometropically