Broadband anti-reflection (AR) coatings are essential elements for improving the photocurrent generation of photovoltaic modules and enhancing visibility in optical devices. In this paper, we report a hybrid-structured, anti-reflection coating that combines multi-layer thin films with a single top-oblique deposited layer. By simply introducing this low-refractive index layer, the broadband anti-reflection properties of optical thin films can be improved while simplifying the preparation. Precise time-controlled and oblique-angle deposition (OAD) methods were used to fabricate the broadband AR coating. By accurately measuring and adjusting the design errors for the thin and thick film layers, 22-layer and 36-layer AR coatings on a sapphire substrate with a 400–2000 nm wideband were obtained. This bottom-up preparation process and AR coating design have the potential to significantly enhance the broadband antireflective properties for many optical systems and reduce the manufacturing cost of broadband AR coatings.