Self-assembly of Au nanoparticles (NPs) coated with positively charged cetyltrimethylammonium ions (CTA(+)) and negatively charged citrate ions in aqueous liquid cell was investigated by in situ transmission electron microscopy (TEM). Under electron illumination in TEM, the hydrated electrons will reduce the overall positive charges of the CTA(+) covered Au NPs and decrease the repulsive electrostatic forces among NPs, leading to assembly of individual NPs into one-dimensional structures. On the contrary, the negatively charged Au NPs coated with citrate ions are steady in liquid cell regardless of electron beam intensity.