Materials formed from micro- and nanoscale particles are of interest because they often exhibit novel optical, electrical, magnetic, chemical, or mechanical properties. In this work, a means of constructing particulate materials using DNA strands to selectively attach micro- and nanoparticles to substrates was demonstrated. Unlike previous schemes, the DNA was anchored covalently to the particles and substrates, rather than through protein intermediaries. Highly reproducible selective attachment of 0.11–0.87 mm-diameter particles was achieved, with selective:nonselective binding ratios >20:1. Calculations showed that at most 350 and 4200 DNA strands were involved in the binding of the small and large particles, respectively. Experiments showed that the DNA was bent at an angle, relative to the surfaces of their solid supports.