Spontaneous, task-free, hemodynamic activity of the brain provides useful information about its functional organization, as it can describe how different brain regions communicate to each other. Neuroimaging studies measuring the spontaneous activity of the brain are conducted while the participants are not engaged in a particular task or receiving any external stimulation. This approach is particularly useful in developmental populations as brain activity can be measured without the need for infant compliance and the risks of data contamination due to motion artifacts. In this project we sought to i) characterize the intrinsic functional organization of the brain in 4-month-old infants and ii) investigate whether bilingualism, as a specific environmental factor, could lead to adaptations on functional brain network development at this early age. Measures of spontaneous hemodynamic activity were acquired in 4-month-old infants (n = 104) during natural sleep using functional near-infrared spectroscopy (fNIRS). Emphasis was placed on acquiring high-quality data that could lead to reproducible results and serve as a valuable resource for researchers investigating the developing functional connectome.