We demonstrate that highly charged, chiral anionic semiconducting polymers helically wrap single-walled carbon nanontubes (SWNTs) at periodic and constant morphology.  These polymers can be used as tools to modulate SWNT electronic properties, provide expansive solubility, or engineer electron acceptor units (e.g., perylene diimide, PDI) at rigorously defined intervals along the nanotube backbone. Femtosecond pump-probe transient absorption spectroscopic experiments show that excitation into the SWNT E₁₁ transition of a S-PBN(b)-Ph₄PDI-[(6,5) SWNT] superstructure generates SWNT hole polaron [(6,5) SWNT^(•+)n] and PDI radical anion (PDI^−•) states.  These studies demonstrate for the first time a photoinduced electron transfer process involving a SWNT and a semiconducting polymer in which: (i) the charge-separated products, and (ii) photoinduced charge separation and thermal charge recombination dynamics, are fully characterized.  To fully exploit these and related polymer-SWNT hybrids in opto-electronic applications, we have developed solution-based processes to structure dense, highly aligned arrays of these nano-objects on solid substrates.  Polyanionic semiconducting polymers designed to wrap SWNTs with a fixed helical screw axis, used in combination with ionic self assembly approaches, enable for the first time the production of functionalized SWNTs that are fully soluble in organic solvents and capable of assembly into complex hierarchical structures that feature aligned nanotubes at high areal density (2.5 x10¹⁰ SWNTs cm^-2) that maintain the opto-electronic properties characteristic of individualized SWNTs.  These porphyrin-polymer/SWNT superstructures can be engineered to undergo both photoinduced electron- and hole-transfer reactions, thereby defining unique energy conversion assemblies, compositions with which to interrogate mechanistic issues regarding photoinduced charge transfer reactions involving nanoscale objects, and utilized as building blocks for highly organized mesoscopic materials that make possible investigation of electron and hole polaron transport phenomena in the solid state, as well as new types of electro-optic materials.