Abstract Ensuring access to clean water remains a global challenge, while conventional contaminant detection and treatment demand high energy. Here, multifunctional metallic nanotube arrays (MeNTAs) engineered with tunable compositions and wettability are reported, enabling self‐powered sensing and thermocatalytic remediation. Ni‐W‐Ni MeNTAs, generating the highest triboelectric voltage, are integrated into droplet‐mode liquid‐solid triboelectric nanosensors (DLS‐TENSs) for detecting Cr 6+ , Pb 2+ , and Hg 2+ , achieving rapid responses within 20 ms. For biological sensing and remediation, superhydrophilic W‐SS MeNTAs are employed. Functionalization with Au nanoparticle‐aptamers allowed highly sensitive E. coli detection, while Bi 2 Te 3 coatings facilitated thermocatalytic H 2 O 2 generation, leading to efficient bacterial inactivation (97%) and Cr 6+ (95%) reduction. To demonstrate practical utility, a wireless sensing bottle is developed for real‐time detection of heavy metals and bacteria in wastewater. Integration of sensing and treatment modules enables simultaneous on‐site monitoring and purification. This work introduces a cost‐effective, portable, and self‐powered platform for advanced water treatment, highlighting the versatility and real‐world potential of MeNTAs.