A series of 100 nm-thick pseudomorphic GaAsBi layers with the Bi content varying from 0.97 to 11.2% have been grown by molecular beam epitaxy (MBE) on the semi-insulating GaAs(100) substrates buffered with an ultra-thin up to 20 nm thick GaAs layer. The main attention in this work was focused on the investigation of relaxation in the Bi induced compressively-strained GaAsBi layers containing a various content of Bi. The lattice parameters of GaAs- Bi compound and the Bi concentration have been evaluated from high resolution X-ray diffraction measurements. The relaxation values of GaAsBi layers ranging from 0.4 to 3.5% were obtained analyzing the symmetric and asymmetric reciprocal space maps of (004) and (115) planes, respectively. Also, the complex study was performed to clarify the relaxation effect on structural, morphological and optical properties of bismide layers. Optical measurements revealed a significant reduction of the energy band gap from 1.34 to 0.92 eV for the layers containing 0.97–8.6% of Bi in the GaAs lattice.