Whole blood viscosity (WBV) is a group of important clinical indicators of cardio-cerebral vascular diseases. Existing detection methods for WBV are complex, making them inconvenient for large population screening. Blood viscosity is closely related to the deformability and aggregation of erythrocytes, which are associated with haemoglobin. Haemoglobin has obvious near-infrared (NIR) spectral absorption. Scattering occurs when NIR light enters a viscous blood sample, and its scattering degree is correlated with blood viscosity. Based on repeated spectral measurements and spectral similarity, spectral noise-to-signal ratio (NSR) was proposed to quantify the spectral scattering effect in the blood sample. A novel selection method of piecewise-continuous wavelengths, named NSR priority-partial least squares (NSRP-PLS), was proposed and applied for visible-NIR quantitative analysis of WBV with high, medium and low shear rates [WBV(H), WBV(M), WBV(L)]. Modelling was separately performed by gender to allow for systematic gender differences in blood viscosity. For the NIR-predicted and clinically measured values of the three WBV indicators in independent validation, the root mean square errors for prediction (SEP) were 0.498, 0.222 and 0.193 (mPa·s), respectively. And the correlation coefficients (RP) were 0.927, 0.934 and 0.927, respectively. Compared with the three current well-performing methods (MW-PLS, CARS-PLS and SPA-PLS), the proposed NSRP-PLS method achieved better predictive accuracy. Results indicated that visible-NIR spectroscopy combined with the NSRP-PLS method can be used for the quantitative analysis of WBV. The proposed analytical method is rapid, reagent-free and is scientific and meaningful for cardio-cerebral vascular diseases screening in large populations.