Preparation from the aqueous alkoxide route of doped and co-doped lithium niobate nanocrystals with Er3+ and Yb3+ ions, and detailed investigations of their optical properties are presented in this comprehensive work. Simultaneous emission under femtosecond laser excitation of second harmonic generation (SHG) and up-conversion photoluminescence (UC-PL) is studied from colloidal suspensions according to the lanthanide ion contents. Special attention has been paid to produce phase pure nanocrystals of constant size (∼20 nm) thus allowing a straightforward comparison and optimization of the Er content for increasing the green UC-PL signals under 800 nm excitation. An optimal molar concentration at about 4 molar% in erbium ions is demonstrated, that is well above the concentration usually achieved in bulk crystals. Similarly, for co-doped LiNbO3 nanocrystals, different lanthanide concentrations and Yb/Er content ratios are tested allowing optimization of the green and red up-conversion excited at 980 nm, and analysis of the underlying mechanisms from excitation spectra. All together, these findings provide valuable insights into the wet-chemical synthesis and potential of doped and co-doped LiNbO3 nanocrystals for advanced applications, combining both SHG and UC-PL emissions from the particle core.