Harnessing chirality can advance diverse technologies, encompassing displays, quantum light sources, secured communication, and biosensing. This thesis explores harnessing chirality in carbon nanotubes (CNTs) at wafer scales, focusing on molecular intrinsic and structurally engineered chirality. Significant advancements were made in alignment techniques, second harmonic generation (SHG) from aligned and chiral CNT films, and engineering structural chirality in CNTs. We developed techniques to enhance CNT alignment using controlled vacuum filtration, including linear reciprocating shaking, and introduced a novel SEM-based method for characterizing nematic order parameters. The AquaGold process was developed for monolayer precision thinning, achieving a wafer-scale aligned CNT film with a thickness of 2.3 nm and a packing factor of 1000 CNTs/μm. Through SHG measurements, we discovered significant second-order optical nonlinearity in wafer-scale, enantiomer-pure, aligned, and densely packed chiral (6,5)- CNT thin films. The only non-zero element of the second-order nonlinear optical susceptibility tensor reached approximately 1.5 nm/V, the highest value for 1D systems. We also fabricated wafer-scale chiral architectures of ordered CNTs with tunable and large circular dichroism. By controlling the stacking angle and handedness, we achieved a high deep-ultraviolet ellipticity of 40 mdeg/nm. These findings pave the way for applications in chiral photonics and opto-electronics.