Ocean alkalinity enhancement (OAE) is a nature-based technology for CO2 removal and storage, but little is known about its environmental safety. We tested a CO2-equilibrated OAE deployment in a close-to-natural community using in situ mesocosms in the oligotrophic subtropical North Atlantic and assessed metazoan zooplankton to inform about food web stability, structure, and production. In addition, a literature review complemented experimental results by summarizing physiological responses of marine animals to decreasing proton concentrations, or increased pH. The food web studied proved resistant, and zooplankton physiologically tolerant, to the OAE tested. We observed short-term effects of OAE on zooplankton reproduction and productivity, which were likely trophically mediated. Yet, these did not affect zooplankton populations or their nutritional value as food for fish. Our study demonstrates an environmentally safe OAE application, but also stresses the risks of more intense OAE options, and the vulnerabilities of other marine ecosystems.