Positron-emission tomography (PET) imaging enables cancer diagnosis at an early stage and to determine its pathological degree. However, tumor uptake efficiency of traditional PET radiotracers is usually low. Herein, we rationally designed a precursor CBT-NODA, the cold analogue CBT-NODA-Ga, and its corresponding radiotracer CBT-NODA-68Ga. Using these three compounds, we verified that coinjection of CBT-NODA-68Ga with CBT-NODA or CBT-NODA-Ga could lead to the synthesis of hybrid gallium-68 nanoparticles in furin-overexpressing cancer cells and enhance microPET tumor imaging in mice. In vivo experiments showed that coinjection of CBT-NODA-68Ga with CBT-NODA-Ga had the most prolonged retention of the radiotracer in blood, the highest radioactivity in tumor regions, and the most enhanced microPET tumor imaging in mice. We anticipate that, by combining the coinjection strategy with our CBT-Cys click condensation reaction, more radiotracers are developed for microPET imaging of more tumors in clinical settings in the future.