Various anisotropic tissue structures exist in organisms, including muscle tissue, skin tissue, and nerve tissue. Replicating anisotropic tissue structures in vitro has posed a significant challenge. 3D printing technology is often used to fabricate biomimetic structures due to its advantages in manufacturing principle. However, direct 3D printing of freeform anisotropic bioactive structures has not been reported. To tackle this challenge, we developed a ternary F/G/P ink system that integrates the printability of Pluronic F127 (F), the robust bioactivity and photocrosslinking properties of GelMA (G), and the shear-induced alignment functionality of high-molecular-weight PEG (P). And through this strategic ternary system combination, freeform anisotropic tissue structures can be 3D printed directly. Moreover, these anisotropic structures exhibit excellent bioactivity, and promote orientational growth of different cells. This advancement holds promise for the repair and replacement of anisotropic tissues within the human body.