between gas and the aqueous solution. [4] Thus, a number of research groups were devoted to designing specific surfaces with specific controllability of bubbles, e.g., superhydrophobic cone, [5] superaerophilic geometry-gradient channel, [6] lubricantinfused slippery surface, [7] elastic liquidinfused material, [8] Janus mesh, [9] etc. Previous studies, to some extent, have realized spontaneous and directional bubble transport underwater, including 1D bubble transport along channels with the assistance of wettability gradient derived from a Janus interconnected structure, [9,10] 2D transport depending on specific inclined planes with the aid of buoyancy or on specific asymmetric surfaces with geometric gradient, [11] demonstrating meaningful but limited bubble transport processes. Further integration of different controlling strategies can diversify the bubble controlling strategy, which should unlock more options for applying such interfaces in extensive fields. [12] For instance, Yong and co-workers demonstrated an effective self-driven gas separation system based on a monolithic photovoltaic-electrolysis device, of which the key idea is gas bubble manipulation by a slippery porous surface and buoyant force. [12b] Zhang et al. incorporated an asymmetric star-shaped slippery track with copper wire cathode, which realized continuous electrolysis and efficient collection of H 2 microbubbles in a pressured environment. [12c] The regulation of bubble transport in aqueous environments is more attractive to broaden the applications of underwater bubble manipulation yet much more challenging because of the increased complexity in dominating bubble transport direction.Water splitting is a promising strategy to produce hydrogen and oxygen synergistically, which is a typical gas-related underwater chemical reaction. [13] The regulation of bubble generation and collection should offer a great opportunity to develop advanced and integrated water-splitting devices toward practical energy production, whereas urgently to be addressed is how to acquire pure product gases. [14] Classical resolutions are introducing ion exchange membranes that prevent the potential gases mixing, but this membrane-based system has demerits in high cost and low durability of membrane modules. [15] Membrane-less electrolysis that gets rid of the membranes from the system and replaces with fluid manipulation to separate the product gases has recently emerged and exhibits superiority Clean energy generated from total water splitting is expected to be an affordable, sustainable, and reliable resource but it remains a challenge to gain pure fuel with a controllable pathway. Here, a simple and economical strategy that enables in situ separation of H 2 /O 2 product by manipulating the generated gas phases with the aid of multi-bioinspired electrodes is proposed. This versatile electrode is based on a Janus asymmetric foam with dual gradients, i.e., the wettability gradient promotes the one-way gas penetration and the geometry gradient boosts the sp...