The design of high-performance complementary meta-resonators for microwave sensors featuring high sensitivity and consistent evaluation of dielectric materials is challenging. This paper presents the design and implementation of a novel complementary resonator with high sensitivity for dielectric substrate characterization based on permittivity and thickness. A complementary crossed arrow resonator (CCAR) is proposed and integrated with a fifty-ohm microstrip transmission line. The CCAR’s distinct geometry, which consists of crossed arrow-shaped components, allows for the implementation of a resonator with exceptional sensitivity to changes in permittivity and thickness of the material under test (MUT). The CCAR’s geometrical parameters are optimized to resonate at 15 GHz. The CCAR sensor’s working principle is explained using a lumped-element equivalent circuit. The optimized CCAR sensor is fabricated using an LPKF protolaser on a 0.762-mm thick dielectric substrate AD250C. The MUTs with dielectric permittivity ranging from 2.5 to 10.2 and thickness ranging from 0.5 mm to 1.9 mm are used to investigate the properties and calibrate the proposed CCAR sensor. A two-dimensional calibration surface is developed using an inverse regression modelling approach to ensure precise and reliable measurements. The proposed CCAR sensor is distinguished by its high sensitivity of 5.74%, low fabrication cost, and enhanced performance compared to state-of-the-art designs, making it a versatile instrument for dielectric characterization.