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Catalysts with designable intelligent nanostructure may potentially drive the changes in chemical reaction techniques. Herein, a multi‐function integrating nanocatalyst, Pt‐containing magnetic yolk‐shell carbonaceous structure, having catalysis function, microenvironment heating, thermal insulation, and elevated pressure into a whole is designed, which induces selective hydrogenation within heating‐constrained nanoreactors surrounded by ambient environment. As a demonstration, carbonyl of α, β‐unsaturated aldehydes/ketones are selectively hydrogenated to unsaturated alcohols with a >98% selectivity at a nearly complete conversion under mild conditions of 40 °C and 3 bar instead of harsh requirements of 120 °C and 30 bar. It is creatively demonstrated that the locally increased temperature and endogenous pressure (estimated as ≈120 °C, 9.7 bar) in the nano‐sized space greatly facilitate the reaction kinetics under an alternating magnetic field. The outward‐diffused products to the “cool environment” remain thermodynamically stable, avoiding the over‐hydrogenation that often occurs under constantly heated conditions of 120 °C. Regulation of the electronic state of Pt by sulfur doping of carbon allows selective chemical adsorption of the CO group and consequently leads to selective hydrogenation. It is expected that such a multi‐function integrated catalyst provides an ideal platform for precisely operating a variety of organic liquid‐phase transformations under mild reaction conditions.

Piezoelectric catalysis has become an emerging research field in recent years, which has received extensive attention. Nanoparticles and nanowires have been developed as piezoelectric catalytic materials. However, in practical research, the use of nanoparticles is not easy for the recovery of samples and will cause secondary pollution, and the current piezoelectric catalysis requires the help of high-frequency ultrasound, which increases the consumption of extra energy and cannot be applied on a large scale. In this study, a self-supporting macroscopic flexible inorganic (Ba,Ca)­TiO3:Pr nanofiber membrane was successfully prepared by electrospinning. Natural energy (water flushing) was used to drive the flexible inorganic (Ba,Ca)­TiO3:Pr nanofiber membrane for piezoelectric catalytic degradation of organic dyes. The results show that the flexible inorganic (Ba,Ca)­TiO3:Pr nanofiber membrane driven by water washing has an obvious piezoelectric catalytic degradation effect on dyes. When the water flow rate was 450 L/h and the concentration of CR solution was 10 mg/L, the catalytic efficiency can reach 91.69%. This study provides a green and feasible method for the preparation of flexible inorganic piezoelectric catalytic materials and the catalytic degradation of organic dyes.