The work below is not mine. It's from user 'Nix' of the Polycount forums. Click on the images to zoom.
He used Blender to model and 3D-paint a character from the game "Bastion." There's no doubt that he used a graphics tablet rather than a mouse for this, to achieve that smooth nuance of tone and texture.
This visual style is worth sharing for reference. In any 3D view, the 3D object looks like a painting. It would look really nice if animated.
Further reading:
• Blender documentation on texture painting: http://wiki.blender.org/index.php/Doc:2.4/Manual/Textures/Painting
• I imagine that this is what Disney's mysterious "Deep Canvas" technology, used on films like Tarzan, is based on: 3D painting that's projected onto models as texture maps. This way the background artists can paint onto 3D models that are used for special animated sequences and composited with 2D animation without breaking the illusion.