I agree with people listing the interrogation scene in TLD. Pure Dalton. Serious, professional and in control. I also will raise the death of Sanchez as one of my key favourite Dalton moments. Banged up, bloodied and exhausted. The best villain death in the series, and I love how Bond broods about it all afterwards.
I definitely agree. I like Sanchez's death because it was very personal and it wasn't like James Bond to do something like this but for some reason it was a nice departure from what we are used to.