The kaolinite sheets were scrolled by sonication-induced chemical delamination processes into well-developed nanotubes (KNs) which were used as substrates for microwave-based ZnO nanoparticles (ZnO/KNs). The biological activities of synthetic ZnO/KNs structures, in terms of the antioxidant and antidiabetic properties, were assessed in comparative studies with the separated phases of the synthetic ZnO and KNs as well as the commercially used ZnO. The KNs substrate resulted in a notable enhancement in the antioxidant and antidiabetic properties of ZnO, which was assigned positive influence on the surface area, interactive interfaces, charge separation, and agglomeration properties of ZnO in addition to the detectable bioactive properties of the KNs structure. The ZnO/KNs structure achieved remarkable scavenging efficiencies for 1, 1-diphenyl-2-picrylhydrazil (DPPH) (89.8 ± 1.57%), nitric oxide (90.6 ± 1.63%), 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS) (86.8 ± 1.28%), and superoxide (43.9 ± 1.72%) radicals. Additionally, it shows high inhibition effects on porcine α-amylase (84.3 ± 1.92%), crude α-amylase (70.6 ± 1.37%), pancreatic α-Glucosidase (94.7 ± 1.54%), crude α-Glucosidase (95.4 ± 1.64%), and amyloglucosidase (95.3 ± 1.32%) enzymes. This antidiabetic activity is significantly higher than the activity of miglitol and close to or slightly higher than acarbose, which leads us to recommend the use of ZnO/KNs when considering the cost and side effects of the commercially used drugs.