Nanodiamonds (NDs) have desirable chemical, physical and biological properties that lend them to a wide range of applications. ND’s facile surface chemistry, for example, can be used to create a high affinity for adsorbing various biological molecules. However, NDs, which are commercially available from multiple vendors, show inconsistencies with surface groups, aggregate sizes and impurity contents that may limit adsorption. We explore adsorption mechanisms of molecules to NDs in efforts to expand ND applications to drug delivery agents, bio-labels and enterosorbents. In doing so, several types of NDs and modification methods are evaluated to increase adsorption capacity and selectivity of propidium iodide and aflatoxin B1. Capacities and binding strengths of target molecules are assessed by Langmuir isotherms and transform calculations. UV-Vis spectroscopy shows our modification treatments are successful in increasing ND adsorption capacities. Additionally, cyclic voltammetry measurements, used to monitor in-situ adsorption, show electrochemical detection even after binding.