A series of Pb(Ti1-xAlx)O3, Pb(Ti1-xNbx)O3 and Pb(Ti1-xAlx/2Nbx/2)O3 thin films were fabricated onto Pt/Ti/SiO2/Si(100) substrates using a chemical solution deposition process. The dielectric constant of the Pb(Ti1-xAlx)O3 thin films increased with increase of aluminum content, while a maximum dielectric constant value was observed for the Pb(Ti1-xNbx)O3 and Pb(Ti1 xAlx/2Nbx/2)O3 thin films when the doping contents were 10 and 20 mol%, respectively. The dielectric constant of the Pb(Ti0.8Al0.1Nb0.1)O3 thin film is about 600, being two times higher than those of Pb(Ti0.9Al0.1)O3 and Pb(Ti0.9Nb0.1)O3 thin films. The Pb(Ti0.8Al0.1Nb0.1)O3 thin film showed less than 10-7 A/cm2 current density at ±150 kV/cm, being superior to the leakage property of the PbTiO3, Pb(Ti0.9Al0.1)O3 and Pb(Ti0.9Nb0.1)O3 thin films. The co-doping of aluminum and niobium is more effective to increase the dielectric and ferroelectric properties as compared with the individual aluminum or niobium doping.