Various methods have been adopted for the high-FF fabrication of MLA. Hexagonal arrays with 100% FF have been demonstrated by self-assembly methods based on dewetting, [7] localized water condensation, [8] or surface wrinkling, [9] but these approaches typically lack control in the design and positioning of the microlenses. In contrast, photolithography techniques have become the gold standard for the production of customized high-FF MLA. [10][11][12][13] Even if unrivaled industrial upscaling is possible, photolithography is optimized for planar substrates and requires multistep processing in expensive clean room facilities. More importantly, the need of masks imposes an additional limit in the degree of tunability of the MLA designs in timely fashion.Alternatively, direct-write technologies (DWTs) such as inkjet printing, [14] microdispensing, [15] two-photon polymerization, [16] laser-induced forward transfer (LIFT), [17,18] or multibeam interferencebased holography [19] enable the direct and maskless fabrication of polymeric microlenses and MLA with perfectly optical quality on a variety of substrates. In this case, though, the use of liquid prepolymers can result in merging of adjacent microlenses that seriously constraints the attainable FF of the arrays. [20] Recent works to improve the FF using DWTs include the fabrication of concave MLA using laser ablation followed by a replica molding step. [21,22] Despite excellent results in terms of uniformity and FF, this approach impedes the direct fabrication of MLA on substrates of interest. Furthermore, most DWTs require complex systems or ultrafast lasers for parallelization, which limit the overall throughput of these systems. Simply put, a low-cost and maskless technique capable of directly generating high-FF arrays at high-throughputs, with controlled geometry and at targeted positions on nonplanar substrates does not exist.In this work, we present a novel laser-based method for the realization of high-FF polymeric microlens arrays that addresses the limitations of traditional direct-write and photolithographic approaches. Our method, termed laser catapulting or LCP, exploits short (in the nanosecond scale) high-energy laser pulses to transfer polymeric solid microdiscs from a uniform film into targeted positions on a receiver substrate. After thermal reflow, namely the heating of the microdiscs above their glass transition temperature (T g ), planoconvex microlenses are obtained. Notably, the direct printing of discs in the solid-state enables the generation of highly close-packed High fill-factor microlens arrays (MLA) are key for improving photon collection efficiency in light-sensitive devices. Although several techniques are now capable of producing high-quality MLA, they can be limited in fill-factor, precision, the range of suitable substrates, or the possibility to generate arbitrary arrays. Here, a novel additive direct-write method for rapid and customized fabrication of high fill-factor MLA over a variety of substrates is demonstrated. This appro...