fields, due to the possibility to fabricate systems and devices featuring micrometer and nanometer resolution. [1][2][3] Among the different technologies, two-photon direct laser writing (DLW) is nowadays one of the best techniques to pattern metallic nanoparticles in complex geometry [4][5][6][7][8][9][10][11] and to nano-fabricate polymeric 3D structures. [12][13][14][15][16][17][18][19][20][21] Briefly, a near infra-red (NIR) ultrafast laser, with high peak power, is tightly focused inside a UV-sensitive photoresist to promote highly localized photochemical reactions through the simultaneous absorption of two (or more) photons. As a third-order non-linear optical process, two-photon absorption (TPA) cross-section depends on the square of the intensity of the laser beam. The polymerization of the liquid-phase precursor is a threshold phenomenon which occurs within the focus figure, inside a sub-micrometric prolate spheroid which defines the smallest printable volume (i.e., voxel). By precisely sweeping the laser focus along the designated path, line by line, 3D microstructures of photocured material are created.Liquid crystals (LCs) have demonstrated a periodically reemerging interest ever since the added value of innovation was introduced when combined with new materials and/or technologies due to their flexibility to self-organize in ordered structures at different scales [22][23][24][25][26][27][28] and their sensitivity to external stimuli. [29][30][31][32][33][34][35][36][37][38] In the field of additive manufacturing by two-photon polymerization (TPP) DLW, the use of mixtures of photopolymers and low molar mass LCs as well as photopolymerizable LCs, also known as reactive mesogens (RMs), paved the way for 3D custom soft photonic devices with tunable properties [39][40][41][42][43][44] and new solutions for micro-robotics. [45][46][47][48][49][50][51] LC elastomers have been employed to fabricate micro-robotic structures, with desired shapes and dimensions, maintaining designed molecular orientation, which can perform reversible shape modification controlled by light. [52][53][54][55][56] TPP-DLW on LCs and monomer mixtures enabled to create electrically controllable complex, multi-dimensional micron-scale structures (i.e., scaffolds) with tunable optical properties. [57][58][59] However, a thorough investigation on the effect of TPP-DLW on the intrinsic properties of the RMs, and on the possibility to deliberately alter them locally in the solidified phase Effective optical elements with tailored properties often rely on the capability to tune the material's structure at the nanoscale. Thanks to their selforganized 1D helical arrangement, cholesteric liquid crystals represent a beautiful example of optical materials whose properties are governed by their supramolecular structure. According to the Bragg's law, selective reflection of circular polarized light occurs for wavelengths within the photonic band gap, which, beside the refractive indices, depends on the helix pitch. Here, polymeric microstructures...