This study examines how recycled, renewable, carbon-sink, and carbon-negative materials can be effectively integrated into modular façade systems—specifically curtain walls and rainscreens—while maintaining performance and constructability standards. A systematic review of English-language literature (2015–2025) retrieved 51 studies that explicitly link alternative materials to modular façade technologies. To compare their diverse metrics, a four-category evaluation framework was developed: Environmental & Climatic Adaptability, Circular Design & Reusability, Constructability & Agility, and Durability & Long-Term Performance. Each paper’s performance metrics—ranging from U-values to reversibility of connections—were mapped, enabling a cross-comparison of technical viability, carbon reduction potential, and readiness levels. Findings reveal that while many studies demonstrate partial alignment with sustainability goals (e.g., reduced embodied carbon or end-of-life recyclability), few address the multifaceted demands of modular façade design, such as ease of disassembly or consistent weather protection. Bio-based and carbon-sink materials, like hemp wool or cork-based panels, show high theoretical viability but require robust fire-safety solutions and stable supply chains. Recycled materials, including thermoplastics and steel scraps, excel in circularity yet often face performance or regulatory barriers. A set of best-practice synergies emerges—e.g., prefabricated timber façade panels integrated with reversible mechanical connections—highlighting potential pathways toward carbon-negative, adaptable building envelopes. The paper concludes by outlining a Climate-Adaptive Design Framework and recommending further exploration of standardizing performance benchmarks and expanding cross-sector collaboration to address technological and regulatory gaps.