Cr3+-doped NH4Al(OH)2CO3 nanotubes, templated by surfactant assemblies, were successfully synthesized via the homogenization precipitation method, and various crystallographic phase Al2O3:Cr3+ nanotubes were also obtained by postannealing at different temperatures. The characteristic R1, R2 doublet line transitions of ruby can be observed in the high crystalline α-Al2O3 nanotubes calcined at temperatures higher than 1200 °C. The results also indicate that the formation mechanism of the tubular nanostructures should result from the self-rolling action of layered compound NH4Al(OH)2CO3 under the assistance of the surfactant soft-template. The convenient synthetic procedure, excellent reproducibility, clean reactions, high yield, and fine quality of products in this work make the present route attractive and significant. Aluminum oxide nanotubes with high specific surface area could be used as fabricating nanosized optical devices doped with different elements and stable catalyst supports of metal clusters.