Results of this study of titanite samples collected from silicate rocks and apatite–nepheline–(sphene) ores from Paleozoic polyphase alkaline nepheline syenite complexes of the Khibiny and Lovozero massifs revealed the possibility of their in-situ U–Pb dating using sensitive high-resolution ion microprobe SHRIMP-II with an accuracy of 1.0–1.5%, which is comparable with that of U–Pb zircon analysis. Employing different approaches to age determination of the formation of the U–Pb system of titanites, the combined isochrons and mixing lines were plotted from the data obtained from the differentiated complex samples (121 analyses of five Khibiny samples and 52 analyses of one Lovozero sample) and apatite–nepheline ores (120 analyses of five Khibiny samples and 88 analyses of three Lovozero samples). They indicate synchronous crystallization of titanite in silicate rocks throughout the complexes: 374.1 ± 3.7 Ma for the Khibiny massif and 380.9 ± 4.5 Ma for the Lovozero massif, and attest to the later formation of phosphate–rare-metal ores: 371.0 ± 4.2 and 361.4 ± 3.2 Ma, respectively. The relatively delayed ore mineralization specific to the Lovozero massif can be accounted for the significantly lower volumes of magmatic melt and ore fluid involved, different thermal conditions, and the pattern of the investigated mineralization. As such, the obtained U–Pb data from titanite make it possible to limit significantly the time interval (most likely, not exceeding 15–20 Ma) comprising the evolution and activity of the ore-magmatic system of major agpaitic complexes, which is probably associated with plume magmatism.