A simple and direct wet chemistry method is reported to simultaneously synthesize nanostructured carbon films and particles through self-assembly of poly(styrene)-poly(4-vinylpyridine) (PS-P4VP) and carbohydrate precursors (turanose, raffinose, alucose, etc.) in two fabrication processes - spin-coating and aerosol processing. Starting with a homogeneous solution containing PS-P4VP and carbohydrates, evaporation of solvent during either spin-coating or an aerosol process leads to the formation of ordered mesostructured films and particles. High temperature treatment in argon atmosphere removes PS fragments, carbonizes carbohydrates and partial PVP fragments, and results in ordered nanoporous carbon films and particles. SEM, TEM, and GISAXS characterization indicates that these nanostructured carbon materials exhibit large nanopores (>20 nm), controlled 1-3 dimensional structures, and controlled surface chemistry. Nitrogen sorption isotherms and electrochemistry characterization indicates the accessibility of the carbon nanopores to both gas phase and aqueous phase. Results suggest that the nanostructured carbon films and particles can be tuned through solvent annealing, precursor concentration, and choice of block copolymers used. These carbon materials present varied practical applications for sorption and separation, sensors, electrode materials, etc.