A selective and sensitive molecular sensor for trivalent lanthanide (Ln(3+)) ions based upon a malonamide-functionalized gold nanoparticle was developed for colorimetric detection in water. A new synthetic approach permits nanoparticle synthesis, stabilization, and incorporation of a selective lanthanide binding site in a single, direct step. The design incorporates a specifically tailored dual function precursor ligand that bears a sodium thiosulfate (Bunte salt) group that links to the gold nanoparticle core and a tetramethylmalonamide (TMMA) group that serves as a selective Ln(3+) binding site. The sensor's colorimetric response to lanthanide ions is immediate, and it is sensitive down to approximately 50 nM for Eu(3+) and Sm(3+). This study demonstrates a general strategy for direct, convenient nanoparticle synthesis that enables the incorporation of analyte binding groups directly to the nanoparticle surface, allowing colorimetric sensors to be developed for widespread use. The one-step synthesis offers uniform surface ligand composition, reduces the volume of waste generated during nanoparticle synthesis and purification, produces functionalized gold nanoparticles that are stable in nonmodified aqueous environments, and offers colorimetric detection at ambient temperature.