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Advancements in wearable electronics and Internet of Things (IoT) sensors have catalyzed the need for effective micro‐energy harvesting. Piezoelectric nanogenerators (PENGs) are ideal due to their high conversion efficiency and durability. However, the contrast between the high piezoelectric coefficients of brittle inorganic ceramics and the lower coefficients of superior flexibility and biocompatibility of organic polymers poses a significant challenge. This work introduces a novel multilayer composite PENG, integrating a single‐crystal BaTiO3 (BTO) film between poly(vinylidene fluoride‐co‐trifluoroethylene) (PVDF‐TrFE) layers. The PVDF‐TrFE/BTO/PVDF‐TrFE PENGs demonstrate substantially improved energy harvesting performance, with outputs reaching up to 15.1 V, 2.39 µA, and power density of 17.33 µW cm−2 during bending deformation. This power density represents a significant increase compared to pure PVDF‐TrFE and nanoparticle BTO‐doped PVDF‐TrFE PENGs. Durability tests show consistent performance, with a stable ∼15.0 V output across 2000 bending cycles. Additionally, when attached to the human body, these PENGs efficiently convert body motions into electrical responses. This work demonstrates a significant enhancement in the performance of PENGs using sandwich‐structured composite of PVDF‐TrFE and freestanding single‐crystal BTO films, showing its potential to address the power requirements of wearable and flexible electronic devices. [ABSTRACT FROM AUTHOR]

• LaB 6 modified sub-nanometer µ-phase strengthening carbon-free FeCoMo steel prepared by SPS technique. • LaB 6 improves the precipitation efficiency of the µ-phase. • LaB 6 inhibits the formation of impurities and reduces their effect on mechanical properties. • FeCoMo steel with 0.2 wt% LaB 6 have excellent hardness, wear resistance and red hardness. LaB 6 -modified carbon-free FeCoMo steels with nano-precipitated phase strengthening have shown excellent sintering and mechanical properties, which enhances their application potential. The results showed that LaB 6 promoted the precipitation of sub-nanometer μ-phase particles from the matrix and reduced the formation of impurity phases during the sintering process. The addition of 0.2 wt% LaB 6 increased the hardness, wear resistance and red hardness of FeCoMo steel by 5.1 %, 26.3 % and 12.6 %, respectively. This study creates conditions for the application of carbon-free FeCoMo steels by introducing LaB 6 to improve their sintering properties and precipitated phase strengthening efficiency. [ABSTRACT FROM AUTHOR]