Silk fibroin (SF) is a natural, degradable, fibrous protein that is biocompatible, is easily processed, and possesses unique mechanical properties. Another natural material, wool keratose (WK), is a soluble derivative of wool keratin, containing amino acid sequences that induce cell adhesion. Here, we blended SF and WK to improve the poor electrospinability of WK and increase the adhesiveness of SF. We hypothesized that microwave-induced argon plasma treatment would improve chondrogenic cell growth and cartilage-specific extracellular matrix formation on a three-dimensional SF/WK scaffold. After argon plasma treatment, static water contact angle measurement revealed increased hydrophilicity of the SF/WK scaffold, and scanning electron microscopy showed that treated SF/WK scaffolds had deeper and more cylindrical pores than nontreated scaffolds. Attachment and proliferation of neonatal human knee articular chondrocytes on treated SF/WK scaffolds increased significantly, followed by increased glycosaminoglycan synthesis. Our results suggest that microwave-induced, plasma-treated SF/WK scaffolds have potential in cartilage tissue engineering.