Due to their fast rates of growth and regeneration, algae are a promising source of biomass for biofuels, aquatic pollution recovery, and a source of protein nutrients, among others. Cultivation of benthic algal biofilm communities, in particular, shows promise for these functions, yet control of quality and yield are strongly dependent on substrata characteristics that affect algal attachment and growth. No previous research efforts have taken advantage of the recent developments in additive technology to support algal biofilm development. Additive manufacturing allows for the design and control of surface features and provides a platform for developing substrata with surface topographies customized for algal colonization. This article seeks to establish the feasibility of colonizing 3D-printed custom substrata with algal biomass. Three exploratory experiments on algal biofilm colonization of printed surfaces were conducted under a variety of laboratory and natural environments, and all printed substrata showed various degrees of colonization success. The preliminary results seem to indicate that (1) 3D-printed substrata can be successfully colonized by algal communities; (2) there is a roughness effect on the colonization rate of benthic algae; (3) substratum roughness can be designed for optimal interstitial spacing between surface asperities, providing refugia for regenerative growth that allows shorter lifecycles of the next algae crop; and (4) increased efficiencies in the packing of biomass can be achieved by complex 3D-printed geometries that provide very high surface area in compact volumes. Future research will seek to quantify these effects as well as to establish substrata conditions that optimize attachment, colonization, and regeneration rates.