Dataset description: raw data for the Nature Structural Molecular Biology paper "A short motif in the N-terminal region of alpha-synuclein plays a critical role in aggregation and function”. Contains raw data corresponding to: • Figure 1, XY data for the in silico aggregation/ solubility analysis of the alpha-synuclein sequence. The algorithm used are also freely accessible online. • Figure 2, XY data for ThT fluorescence assays with WT, delta P, delta P2 and delta delta synuclein variants under different buffer conditions. • Figure 3, XY data for ThT fluorescence assays of different cysteine variants of disulphide locked, dimeric alpha-synuclein • Figure 4, intensity ratios of paramagnetic: diamagnetic data from PRE NMR experiments for WT alpha-synuclein, presented as XY data. • Figure 5, intensity ratios of paramagnetic: diamagne tic data from PRE NMR experiments for delta delta alpha-synuclein, presented as XY data. • Figure 6, raw data of the number of mobile and immobile inclusions larger than ~2µm2 per animal between the tip of the nose and pharyngeal bulb during ageing determined using FRAP. Additionally, raw data of Number of body bends per second (BBPS) of N2, WT aSyn::YFP, ?P1::YFP and ??::YFP animals from Day 0 (L4 stage) through to Day 13 of adulthood. • Figure 7, Raw XY MRE values from CD experiments of WT, delta delta and deltaP1 deltaP2 variants at different concentrations of DMPS liposomes. Additionally, XY data for ThT fluorescence assays of WT, delta delta and deltaP1 deltaP2 variants incubated with different concentrations of DMPS liposomes. • Figure 8, Raw intensity ratios (in presence: absence of liposomes) of WT and delta delta alpha-synuclein from 1H-15N HSQC NMR experiments. • Figure S1, XY data for ThT fluorescence assays with WT, delta P1, delta P2 and delta delta synuclein variants under different buffer conditions. • Figure S2, XY data for ThT fluorescence assays with WT alpha-synuclein in seeding conditions. • Figure S3, XY data for ThT fluorescence assays with WT, P1P2GS and delta C1 control synuclein variants under different buffer conditions.< /li> • Figure S4, see data for Figure 4. • Figure S5, HN-G2 rates for WT aSyn labelled with MTSL at position 40 (A40C) and WT and delta delta variants labelled with MTSL at position 129 (A129C). • Figure S6, see figure 7 for raw CD MRE data. Raw DLS data presented as XY data.