Developing photocatalytic technologies for pollutants removal with high harmless product selectivity is a significant challenge. Construction and optimization of nanocomposites junction with appropriate band alignments is an effective method for achieving this objective. Herein, a unique popcorn-stick-like NH2-UiO-66/TiO2 nanotube nanocomposites with staggered band alignment is fabricated. The small metal organic frameworks (MOFs) particles with diameters around 20 nm are uniformly dispersed on the surface of TiO2 nanoplates, creating a popcorn-stick-like structure. The resulting as-synthesized nanocomposites photocatalysts show distinguished photocatalytic activity for simultaneous removal of carbon particles and nitrogen dioxide with 100% NO2 conversion and 99% N2 selectivity, about 3.9 times higher than that of pristine TiO2. The significant enhancement is attributed to the rapid charge separation and transfer in TiO2 and NH2-UiO-66 interface and the visible light absorption. The enhanced charge transfer follows double charge transfer mechanism, which is confirmed by surface photovoltage spectroscopy, photoluminescence, transient photocurrent measurements, and electrochemical impedance spectroscopy. This study demonstrates the potential for the simultaneously removal of two pollutants using the composite of TiO2 and MOF materials with high surface area and visible light absorption ability, thereby providing the possible applications of NH2-UiO-66/TiO2 composites in environmental remediation including air purification and wastewater treatment.