A deuterium-deuterium neutron generator device based on the 2.45-GHz electron cyclotron resonance technique has been designed. The device achieves a neutron yield of 5 × 108 n/s supplied by the ion source with a beam current of 5 mA. The device is intended for use in radiation modification, isotope production, prompt gamma neutron activation analysis, and boron neutron capture therapy studies. In this work, we study the effects of stainless steel, glass, and aluminum (Al) chamber linings with boron nitride (BN) and glass front plates on both the ion source–induced beam quality and the neutron source yield. The results show that the combination of an Al chamber liner with a BN front plate liner increases current and neutron yield by three to four times compared to other combinations. Stable Al2O3 films generated on the Al surface in air, as confirmed by X-ray diffraction pattern analysis, have a high secondary electron emission coefficient and low wall recombination coefficient, which contributes to the generation of D+ ions in the chamber. As a result, the ion source current and neutron generator yield are improved.