Additional experimental details and methods, including sample preparation, calculation methods; single-crystal images; polarized Raman spectrum of NbOBr2; layer-dependent Raman spectra; details of the bending-substrate method; repeated experiments; strain-polarized SHG spectra for NbOBr2; thickness measurement of strained NbOBr2 samples; and calculated slopes of bond length variation of NbOBr2 under strain.