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• Cytocompatible bacterial ATRP (b- ATRP) was developed. • Bacterial nanohybrids with high viability were obtained with b -ATRP. • The surface electric property of bacterial cells was well-controlled by b- ATRP. • Cr(VI) removal rate was improved by 3 times with bacterial nanohybrid. Surface-initiated activator regenerated by electron transfer atom transfer radical polymerization (SI-ARGET ATRP) has great potential to modify living cell surface with controlled architecture and tailored phenotype. However, it is challenging to engineer the bacterial cells with current SI-ARGET ATRP due to low cellular tolerance to the toxic reagents in polymerization. In this study, a cytocompatible bacterial SI-ARGET ATRP (b -ATRP) strategy was developed for individual nanoencapsulation of living bacterial cell. With step by step optimization of reaction conditions, living nanohybrid with high cell viability (>70%) was achieved with b -ATRP. Furthermore, living Shewanella nanohybrids with controllable surface electric property were fabricated with b -ATRP and applied for aqueous Cr(VI) treatment. Impressively, nanoencapsulation of cells with poly(4-vinylpyridine) improved the Cr(VI) removal rate by 3 times. This work provided a new approach to engineer the living bacterial cell surface and expanded the ATRP applications to prokaryotic cell and bioremediation. [ABSTRACT FROM AUTHOR]