Dietary sodium (Na) levels were related to the content of the eggshell matrix. We therefore speculated that dietary Na supplementation as sodium bicarbonate (NaHCO3) or sodium sulfate (Na2SO4) may improve eggshell quality. Additionally, dietary NaHCO3 or Na2SO4 supplementation may further affect eggshell quality in different ways due to differences in anions. This study investigated and compared the effects of dietary Na supplementation in either NaHCO3 or Na2SO4 form on laying performance, eggshell quality, ultrastructure and components in laying hens. A total of 576 29-week-old Hy-Line Brown laying hens were randomly allocated to 8 dietary treatments that were fed a Na-deficient basal diet (0.07% Na, 0.15% Cl) supplemented with Na2SO4 or NaHCO3 at 0.08, 0.18, 0.23 or 0.33% Na for 12 weeks. No differences were observed in laying production performance with dietary Na supplementation. Dietary Na supplementation resulted in quadratic increases of eggshell breaking strength in both Na2SO4 and NaHCO3 added groups (P < 0.05), and Na2SO4-fed groups had a quadratic increase in the eggshell ratio at week 12 (P < 0.05). Compared with supplementing 0.08% Na, dietary supplementation of 0.23% Na increased the effective thickness (P < 0.05) in both Na2SO4 and NaHCO3 added groups, but decreased the thickness and knob width of the mammillary layer (P < 0.05). A linear increase on the calcium content of the shell was only observed with Na supplementation from NaHCO3 (P < 0.05). No differences were observed in Na contents of the shell with dietary Na supplemented by both sources. Dietary Na addition had a quadratic increase on uronic acid contents of shell membrane in NaHCO3-fed groups (P < 0.05). Moreover, the sulfated glycosaminoglycan (GAG) contents of shell membranes increased linearly with dietary Na supplementation (P < 0.05). Dietary supplementation of 0.23% Na from Na2SO4 increased the sulfated GAG contents of calcified eggshell (P < 0.05). Additionally, compared with NaHCO3-fed groups, Na2SO4-fed groups had higher eggshell breaking strength, thickness, eggshell weight ratio, effective thickness and the sulfated GAG contents of calcified eggshell at week 12. Overall, dietary supplementation of NaHCO3 or Na2SO4 could increase eggshell breaking strength, which may be related to increased sulfated GAG contents in eggshell membranes and improved ultrastructure. Higher eggshell breaking strength, thickness and eggshell ratio could be obtained when the diet was supplemented with 0.23% Na from Na2SO4.