Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (<i>D</i><sub>c</sub>) distribution with very thin coating thickness throughout the detectable range of <i>D</i><sub>c</sub>. However, the size distribution of <i>D</i><sub>c</sub> (project average mass median <i>D</i><sub>c</sub> = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BC<sub>tr</sub>) and from SF (BC<sub>sf</sub>), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BC<sub>tr</sub> and BC<sub>sf</sub> showed distinctly different <i>D</i><sub>c</sub> distributions and coating thicknesses, with BC<sub>sf</sub> displaying larger <i>D</i><sub>c</sub> and larger coating thickness compared to BC<sub>tr</sub>. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC–AMS–PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). <br><br> Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BC<sub>sf</sub> fractions that ranged from low to high, and whose mass median <i>D</i><sub>c</sub> values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core – <i>D</i><sub>p</sub>/<i>D</i><sub>c</sub>) for these same sectors was 1.28 ± 0.07, 1.45 ± 0.16 and 1.65 ± 0.19. For W, SE and E air masses, the number fraction of BC<sub>sf</sub> ranged from 6 ± 2% to 11 ± 5% to 18 ± 10%, respectively, but importantly the larger BC core sizes lead to an increased fraction of BC<sub>sf</sub> in terms of mass than number (for W, SE and E air masses, the BC<sub>sf</sub> mass fractions ranged from 16 ± 6%, 24 ± 10% and 39 ± 14%, respectively). An increased fraction of non-BC particles (particles that did not contain a BC core) was also observed when SF sources were more significant. The BC mass attribution by the SP2 method agreed well with the BC–AMS–PMF multiple linear regression method (BC–AMS–PMF : SP2 ratio = 1.05, <i>r</i><sup>2</sup> = 0.80) over the entire experimental period. Good agreement was found between BC<sub>sf</sub> attributed with the Aethalometer model and the SP2. However, the assumed absorption Ångström exponent (α<sub>wb</sub>) had to be changed according to the different air mass sectors to yield the best comparison with the SP2. This could be due to influences of fuel type or burn phase.