The pollution of the marine environment with plastic debris is expected to increase, where ocean currents and winds cause their accumulation in convergence zones like the North Pacific Subtropical Gyre (NPSG). Surface-floating plastic (>330 μm) was collected in the North Pacific Ocean between Vancouver (Canada) and Singapore using a neuston catamaran and identified by Fourier-transform infrared spectroscopy (FT-IR). Baseline concentrations of 41,600–102,700 items km–2 were found, dominated by polyethylene and polypropylene. Higher concentrations (factors 4–10) of plastic items occurred not only in the NPSG (452,800 items km–2) but also in a second area, the Papaha̅naumokua̅kea Marine National Monument (PMNM, 285,200 items km–2). This second maximum was neither reported previously nor predicted by the applied ocean current model. Visual observations of floating debris (>5 cm; 8–2565 items km–2 and 34–4941 items km–2 including smaller “white bits”) yielded similar patterns of baseline pollution (34–3265 items km–2) and elevated concentrations of plastic debris in the NPSG (67–4941 items km–2) and the PMNM (295–3748 items km–2). These findings suggest that ocean currents are not the only factor provoking plastic debris accumulation in the ocean. Visual observations may be useful to increase our knowledge of large-scale (micro)plastic pollution in the global oceans.