State of the surface: 2D photoactive materials may offer interesting opportunities in photocatalytic devices. Unfortunately, high-surface-area 2D photo-electrodes made from nanosheets self-assembly usually suffer from poor charge carrier transport and high recombination on surface states. In this study, high solar H2 photocurrents up to 4.5 mA cm−2 are achieved on p-WS2 resulting from the careful design of the film nanostructure and use of a healing catalyst promoting surface states chemical modification. Large scale development of the 2D transition metal di-chalcogenides (TMDC) relies on landmark improvement in performance, which could emerge from nanostructuration. Using p-WS2 nanoflakes with different degrees of exfoliation and fracturing, perspectives were provided to develop high-surface-area 2D p-WS2 films for the photocatalytic hydrogen generation. The critical role of inter-nanoflakes contacts within high-surface-area 2D films was demonstrated, highlighting the benefit of plane/plane versus edge/plane contacts. Evidence of the high density of surface states displayed by these 2D films was provided through electrochemical measurements. In addition to operating as recombination centers, the surface states were shown to give rise to deleterious Fermi-level pinning (FLP), which dramatically decreased the efficiency of charge carrier separation. Lastly, promising strategies yielding FLP suppression via surface states modification were proposed. In particular, use of a multifunctional ultrathin film displaying healing, catalytic, and n-type semiconduction properties was shown to greatly enhance charge carrier separation and transport to the photo-electrode/electrolyte interface. When the 2D photoelectrodes were fabricated with the above prerequisites (i. e., a high proportion of plane/plane contacts and a successful surface states chemical modification), a photocurrent up to 4.5 mA cm−2 was achieved for the first time on 2D p-WS2 photocathodes for hydrogen generation.