Hybrid systems that integrate synthetic materials with biological machinery offer opportunities for sustainable and efficient catalysis. However, the multidisciplinary and unique nature of the materials-biology interface requires researchers to draw insights from different fields. In this Perspective, using examples from the area of N2 and CO2 fixation, we provide a unified discussion of critical aspects of the material-microbe interface, simultaneously considering the requirements of physical and biological sciences that have a tangible impact on the performance of biohybrids. We first discuss the figures of merit and caveats for the evaluation of catalytic performance. Then, we reflect on the interactions and potential synergies at the materials-biology interface, as well as the challenges and opportunities for a deepened fundamental understanding of abiotic-biotic catalysis.