The boundary layer flow of an incompressible viscoelastic Jeffrey’s nanofluid from a vertical permeable flat plate is investigated. We consider the effects of heat generation, thermal radiation, and chemical reaction on the fluid flow. The nonlinear transformed coupled differential equations that describe the transport processes are solved numerically using a multidomain bivariate spectral quasilinearization method (MD-BSQLM). This innovative method involves blending the quasilinearization idea with the bivariate Lagrange interpolation. The solutions of the resulting system of equations are then obtained sequentially on multiple intervals using the Chebyshev spectral collocation method. The method is shown to give accurate solutions for boundary layer-type equations. The influence of various physical parameters on velocity, temperature, and nanoparticle concentration fields, as well as on the skin friction and heat and mass transfer coefficients, is shown and discussed in detail. The range of the values of the governing parameters considered in this study is between 0 , 4 . For qualitative validation of the results and the numerical method used, calculations were carried out to graphically obtain the velocity, temperature, and nanoparticle concentration fields for selected physical parameter values. The results obtained were found to correlate with the results from published literature. For quantitative verification of our findings, the MD-BSQLM numerical solutions were again confirmed against published results reported in the literature, and the results were observed to be in perfect agreement. This study’s findings indicate that the Deborah number and suction parameter have related effects on the velocity profile, which is to suppress both the flow velocity and the momentum boundary layer thickness. Increasing the heat generation and thermal radiation parameters enhances both the temperature and thermal boundary layer depths. In contrast, an increase in the chemical reaction parameter causes a decrease in the fluid concentration.