The inherent strength of individual carbon nanotubes (CNTs) offers considerable opportunity for the development of advanced, lightweight composite structures. Recent work in the fabrication and application of CNT forms such as yarns and sheets has addressed early nanocomposite limitations with respect to nanotube dispersion and loading and has pushed the technology toward structural composite applications. However, the high tensile strength of an individual CNT has not directly translated into that of sheets and yarns, where the bulk material strength is limited by intertube electrostatic attractions and slippage. The focus of this work was to assess postprocessing of CNT sheets and yarns to improve the macro-scale strength of these material forms. Both small-molecule functionalization and electron-beam irradiation were evaluated as means to enhance the tensile strength and Young's modulus of the bulk CNT materials. Mechanical testing revealed a 57% increase in tensile strength of CNT sheets upon functionalization compared with unfunctionalized sheets, while an additional 48% increase in tensile strength was observed when functionalized sheets were irradiated. Similarly, small-molecule functionalization increased tensile strength of yarn by up to 25%, whereas irradiation of the functionalized yarns pushed the tensile strength to 88% beyond that of the baseline yarn.