Silks spun by the arthropods are "ancient' materials historically utilized for fabricating high-quality textiles. Silks are natural protein-based biomaterials with unique physical and biological properties, including particularly outstanding mechanical properties and biocompatibility. Current goals to produce artificially engineered silks to enable additional applications in biomedical engineering, consumer products, and device fields, have prompted considerable effort towards new silk processing methods using bio-inspired spinning and advanced biopolymer processing. These advances have redefined silk as a promising biomaterial past traditional textile applications and into tissue engineering, drug delivery, and biodegradable medical devices. In this review, we highlight recent progress in understanding natural silk spinning systems, as well as advanced technologies used for processing and engineering silk into a broad range of new functional materials.