As an important method of enriching, separating and removing nanoparticles, colloidal gas aphrons (CGAs) need to be investigated for the fate and interfacial behaviors of particles during the process. It is beneficial to sufficiently interpreting the process performance and mechanisms. This study employed complementary tracking technologies to analyze the extensively-used engineered nanoparticles - TiO2 nanoparticles (TiO2-NPs) in effluent and floats of CGA process. Results denote that, at the optimum SDS relative dosage of 0.78mg/mg TiO2, the particle number concentration was largely reduced by 2-4 orders of magnitude based on nanoparticle tracking analysis (NTA) whilst approximately 84.0% of TiO2-NPs were separated according to inductively coupled plasma-mass spectrometry (ICP-MS). NTA shows the change of overall particle dispersion status in the water phase while ICP-MS provides the Ti-related separation effect. Particularly, the particle size variation for the scenario of overdosing CGAs was clearly observed by NTA. Micro-Raman, dynamic laser scattering and small angle laser light scattering exhibited advantages in obtaining the configuration and morphology of flocs. The large flocs with open structure were apt to form and be favorably separated at the appropriate CGA dosage. However, overdosing CGAs weakened the capture capacity of bubbles and gave rise to small and dense aggregates. This work, for the first time, shows the change of nanoparticles in water and solid phases using the important and novel nanoparticle collection method - CGA technology. It also provides a reference to other flotation-related technologies for studying the nanoparticle fate and the process performance.