This study presents a significant advancement in LED interior lighting through the development and application of Asymmetric Lens–Total Internal Reflection (AL–TIR) optics, with a focus on enhancing lighting uniformity and indoor comfort by simulating sky-like lighting distribution. AL–TIR technology employs asymmetric lenses combined with total internal reflection to efficiently redirect and spread light, achieving a controlled and even ceiling illumination suitable for various interior applications. This research explored the establishment of ideal luminous intensity curves, devised practical AL–TIR optical designs through numerical calculations, and conducted extensive simulations to assess performance in typical indoor environments. Our findings demonstrated substantial improvements in lighting uniformity, with the AL and AL–TIR systems achieving direct illuminance uniformities of 0.78 and 0.83, respectively, compared to traditional tube LEDs at 0.25. These results, validated in several office rooms, highlight the efficacy of AL–TIR optics in revolutionizing indoor lighting design by balancing optimal lighting distribution with occupant comfort and well-being.