A series of unique flake-tube structured p-n heterojunctions of BiOI/TiO2 nanotube arrays (TNTAs) were successfully prepared by loading large amounts of BiOI nanoflakes onto both the outer and inner walls of well-separated TiO2 nanotubes using anodization followed by the sequential chemical bath deposition (S-CBD) method. The as-prepared BiOI/TNTAs samples were characterized by X-ray diffraction, electron microscopy, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance spectroscopy and nitrogen sorption. The photoelectrocatalytic (PEC) activity and stability of the BiOI/TNTAs samples toward degradation of methyl orange (MO) solutions under visible-light irradiation (λ > 420 nm) were evaluated. The visible-light PEC performance of BiOI/TNTAs samples was further confirmed by the transient photocurrent response test. The results from the current study revealed that the 5-BiOI/TNTAs sample exhibited the best PEC activity, favourable stability, and the highest photocurrent density among all the BiOI/TNTAs heterostructured samples. The combined effects of several factors may contribute to the remarkable visible-light PEC performance for the 5-BiOI/TNTAs sample including a 3D connected intertube spacing system and an open tube-mouth structure, strong visible-light absorption by BiOI, the formation of a p-n junction, larger specific surface area, and the impact of the applied external electrostatic field.