Intermittency is widely observed in various nonlinear dynamical systems as an intriguing transient dynamic far from equilibrium. The internal dynamics formed by a pair of interacting optical solitons are often analogized to typical nonlinear systems. However, whether intermittency exists within the intramolecular motion remains to be investigated. Here, we study the intermittent dynamics of soliton molecules in ultrafast lasers, employing balanced optical cross-correlation techniques with sub-femtosecond temporal resolution. We demonstrate the occurrence of the bursting phase of intense variations of pulse separation within regular breather rhythms. In addition, we discover the intermittent transitions route to chaotic soliton molecules, facilitated by gain control. A series of analysis methods are used to assess the chaotic signals, providing compelling experimental evidence that soliton molecules can be analogized to their matter molecule counterparts. Our experimental findings shed light on the non-equilibrium intramolecular dynamics, providing insight into the transition of the attractors within interacting dissipative solitons in laser and fiber resonators.