There are many ways to define "smooth", and only you know which definition fits your needs. But, anyway, here are a few things to think about.
The typical mathematical definition of "smooth" says something about how many continuous derivatives the function has. But these sorts of definitions bear little relationship to the intuitive notion of "smoothness" of a curve. Polynomial curves are $C^\infty$, but, as you noted, if they are constructed by Lagrange interpolation, they often wiggle all over the place, and no-one (except a mathematician) would call them "smooth". Also, any statement about continuity of derivatives is dependent on the parameterization of the curve, whereas smoothness is usually considered to be a purely geometric property that is independent of parameterization.
There are numerous techniques for improving curve smoothness by minimizing some "energy" function. The idea is that the curve is analogous to a thin beam, which will try its best to assume a smooth shape by "relaxing" its internal energy. As the other answer pointed out, cubic splines are based on one such energy minimization idea. In fact, before mathematicians started studying them, "splines" were thin strips of wood used to define smooth shapes for ship hulls and aircraft fuselages. One reference is here, but you can find many others by searching for the term "minimum energy spline".
Another idea, common in product design, is that a curve is "smooth" if its curvature varies in some very simple way. Nice-looking curves either have monotone curvature, or a curvature function that has a single maximum. So, from this point of view, the smoothest curves are straight lines and circular arcs. Conic section curves are also popular in design, since their curvature functions are simple and predictable.
Carlo Sequin and his students have studied "MVC" curves (minimum variation of curvature). See the list of papers here, and especially Henry Moreton's thesis.
A curve whose curvature is a linear function of arclength is an Euler spiral. There is a nice thesis by Raphael Levien that discusses these types of curves and related topics.