Figure S1 and Video S1, Supporting Information). Vessel-damage-free deployment requires the shape recovery of a graft through circumferential tube expansion by ≈40%-50% to fit the host vessel after insertion (Videos S1-S3, Supporting Information). Hence, a new class of shape memory polymer (SMP) library was synthesized through ring opening polymerization [3] with ε-caprolactone (CL) and glycidyl methacrylate (GMA) monomers (Figure 1a; Figure S2, Supporting Information). Vessel property-matching optimization necessitated a combinatorial design strategy [4] to produce tunable SMP properties through a series of development steps (Figure 1b-g). First, the idea of decreasing the shape recovery temperature, which was represented by melting temperature (T m ), to the body temperature range was validated [5] by the differential scanning calorimetry (DSC) (Figure 1b). T m decreased from the temperature of the base poly(ε-caprolactone) (PCL) to that of our SMPs because crosslinking reduced the crystallinity of PCL. This effect was more dominant compared to the increase in the tightness of the polymer chains owing to Inserting a graft into vessels with different diameters frequently causes severe damage to the host vessels. Poor flow patency is an unresolved issue in grafts, particularly those with diameters less than 6 mm, because of vessel occlusion caused by disturbed blood flow following fast clotting. Herein, successful patency in the deployment of an ≈2 mm diameter graft into a porcine vessel is reported. A new library of property-tunable shape-memory polymers that prevent vessel damage by expanding the graft diameter circumferentially upon implantation is presented. The polymers undergo seven consecutive cycles of strain energy-preserved shape programming. Moreover, the new graft tube, which features a diffuser shape, minimizes disturbed flow formation and prevents thrombosis because its surface is coated with nitric-oxide-releasing peptides. Improved patency in a porcine vessel for 18 d is demonstrated while occlusive vascular remodeling occurs. These insights will help advance vascular graft design. Biomedicine