Innovative methods to lower arsenic (As) exposure are sought. The As regulatory protein (ArsR) is reported of having high affinity and specificity to arsenite [As(III)]. Rhodopseudomonas palustris CGA009 is a good model organism for studying As detoxification due to at least three ars operons and four diverse arsR (RP1-4) on the genome. In this study, four Escherichia coli harboring arsR (RP1-4) derived from CGA009 were engineered and tested regarding their As resistance. The results showed that E. coli (arsR (RP2)) displayed robust As(III) resistance, and its growth inhibition rate was only 2.9% when exposed to 3.0 mmol/L As(III). At pH 7.0, E. coli (arsR (RP2)) showed an enhanced As adsorption capacity. As(III) (2.32 mg/g (dry weight, dw)) and 1.47 mg/g arsenate [As(V)] was adsorbed representing a 4.2-fold and 1.3-fold increase respectively compared to the control strain. The adsorption process was well fitted to Langmuir isothermal mode. E. coli (arsR (RP2)) (1.0 similar to 12.0 g/L) could remove 30.3 similar to 82.2% of As (III) when exposed to 10 mu g/L As(III). No increase in absorption to copper(II), zinc(II), chromium(III), and lead(II) could be detected. Our studies revealed that arsR (RP1-4) from CGA009 could confer As(III) resistance; E. coli (arsR (RP2)) displayed the highest As resistance, selectivity, and adsorption capacity within a wider pH (5.0 similar to 9.0) and salinity (0 similar to 15.0 g/L NaCl) range, especially important as it could remove As(III) from low concentration As-containing water.