important functions of wearable devices. Since flexible pressure sensor converts external stimuli into electrical signals and can be processed into various shapes, it displays indispensible applications in robots, wearable individual-centered health monitoring, sensitive tactile information acquiring, prosthetics, etc. [4][5][6][7] In general, such sensors contain a number of circuits or complex layered matrix arrays, as reported in the excellent works by Bao's group. [5,[7][8][9][10] From the utilized physical effects and compositions, most of the current flexible sensors are capacitors, [8,[11][12][13] piezoresistors, [14][15][16][17] and triboelectricity. [18][19][20][21] Flexible piezoelectric sensor attracted much attention due to its high sensitivity, simple structure, and easy data processing. [22,23] Up to now, many micro/ nanostructure piezoelectric materials such as ZnO nanowires, [24] BaTiO 3 nanowires, [25][26][27] PZT nanowires, [28] PbTiO 3 / ZnO nanobrush, [29] GaN nanowires, [30] Ge/ Si nanowires, and PZT nanorod arrays have demonstrated high sensitivity in electrical responses under small external pressure regimes. [26,[31][32][33][34] These nanostructured piezoelectric shapes with high anisotropy have displayed high sensitivity because of easier deformation under external forces. However, the syntheses of nanowires, nanorods, and nanobrushes are usually complicated, expensive, and less productive. BaTiO 3 (BT) piezoelectric microplatelets show a largely anisotropic structure, and can be easily synthesized into micrometer-sized single crystal platelets with controllable morphologies and high yields by topological chemistry technology in molten salt synthesis. [35][36][37][38][39] The BT single-crystal microplatelets were widely used as templates to induce (00l) textures in PMN-PT, PMN-PZT, and PIN-PMN-PT ceramics, so that high electromechanical properties could be achieved in these textured piezoceramics. [36,[40][41][42][43][44][45] Furthermore, the anisotropic microplatelets have also been applied to reinforce and toughen the polymer-based composite materials. [46,47] Kotov and co-workers [47] reported a polyvinyl alcohol (PVA)/ montmorillonite (MTM) composite, in which nanosize MTM platelets were orderly aligned by using a layer-by-layer (LBL) self-assembly process. An ultra-enhanced strength was reached in the organic-inorganic hybrid PVA/MTM composite film.Piezoelectric wearable electronics with flexibility and high sensitivity have received increasing attention in the fields of health monitoring, flexible robots, and artificial intelligence. Here, a flexible organic-inorganic hybrid composite for wearable electronics application based on (00l)-aligned BaTiO 3 (BT) single-crystal microplatelets is prepared by layer-by-layer self-assembly technology. For the polyvinylidene fluoride-trifluoroethylene (P(VDF-TrFE))/BT single-crystal microplatelets composite film, the sensitivity is nearly 20 times higher than that of its counterparts of P(VDF-TrFE)/BT microparticles composite film and pure P(VD...