Plasmonic sensing based on nanostructures is a powerful analytical tool for ultrasensitive label-free biomolecule detection that holds great potential in the field of clinical diagnostics and biomedical research. Here, we report the fabrication, the characterization, and the principle of operation of gold nanorod hyperbolic metamaterials (NHMMs) along with ultrasensitive bulk refractive index and label-free biomolecular detection. By combining electron-beam lithography and nanoscale electroplating, we demonstrate the fabrication of a highly ordered, height-controllable, and vertical array of nanorods. By exciting the bulk plasmon–polariton mode in the NHMM using a prism-coupling technique and integrating the sensor in microfluidics, we demonstrate that the bulk sensitivity and figure of merit of our device could reach 41,600 nm/RIU and 416 RIU^-1, respectively. The physical mechanism of this high bulk sensitivity is revealed through theoretical and experimental studies. Moreover, by bio-functionalizing the surface of the NHMM sensor, monitoring the binding of streptavidin at dilute concentrations is performed in real time. We test different concentrations of streptavidin ranging from 200 to 5 µg/mL, and the NHMM biosensor exhibits a 1 nm wavelength shift for a 5 µg/mL streptavidin detection. By fitting the Hill equation of the NHMM biosensor and taking into account the level of noise (0.05 nm) as the minimum wavelength shift of the detectable limit, the limit of detection of the NHMM biosensor to streptavidin can be estimated to be 0.14 µg/mL (2.4 nm). As a direct comparison, a 0.5 nm wavelength shift for 20 µg/mL of streptavidin is reported when using a conventional gold film sensor under identical experimental conditions. The developed plasmonic NHMM sensor shows tremendous potential for highly sensitive bulk solutions and biomolecule detection and provides a promising avenue for free-label biosensing applications in the future.