Square‐Wettability Patterned, Recyclable Polyolefin Elastomer Sorbents for Efficient Chemical and Oil Spill Collection

Effective remediation of marine chemical spills remains a critical challenge due to the rapid dispersion and volatility of hazardous compounds. Conventional polypropylene (PP) sorbents exhibit limited absorption kinetics and pose risks of secondary contamination. Here, an architected polyolefin elastomer (POE) film is presented with engineered surface macro‐patterns that enhance solvent uptake via polymer matrix swelling in the amorphous phase. Pattern spacing is systematically tuned to regulate sorption dynamics and film–solvent interactions. The optimized POE film achieved a chloroform uptake of 36.2 g g −1 within 10 min—surpassing commercial PP sorbents (14.2 g g −1 ) and unpatterned POE films (19.7 g g −1 ). Finite element modeling corroborated that sorption behavior is governed by film thickness and surface geometry. Additionally, functionalization with magnetic nanoparticles enabled facile recovery, while fluorescence doping facilitated nighttime detection. Importantly, the all‐polyolefin composition permits complete recyclability through standard pyrolysis pathways, aligning with crude oil refining streams. This multifunctional, recyclable sorbent platform offers a promising avenue for responsive, high‐performance, and sustainable environmental protection technologies.