This thesis examines the synthesis of metal-free organic dyes for light-harvesting applications within the DSSC manifold. All DSSC organic dyes possess a similar donor-π-spacer-acceptor (D-π-A) motif. Here, triphenylamine (TPA) is employed as a donor owing to its redox stability and cyanoacetic acid has been utilized as an acceptor due to its electron-withdrawing ability. Thiophenes are ubiquitous in organic materials chemistry owing to their exceptional charge transport behavior, and in this body of work, π-spacers incorporating benzodithiophene and thiophene-quinones have been incorporated into a DSSC dye and their utility explored. Fused thiophene cores are non-innocent π-spacers. Non-innocent, in this context, is defined as π-spacers that incorporate a secondary chromophore or redox active species (benzodithiophene or quinone).